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Human health risks estimations from polycyclic aromatic hydrocarbons in serum and their hydroxylated metabolites in paired urine samples
2021
Yang, Ziying | Guo, Chongshan | Li, Qin | Zhong, Yi | Ma, Shengtao | Zhou, Jinhua | Li, Xiaotong | Huang, Rende | Yu, Yingxin
Polycyclic aromatic hydrocarbons (PAHs) are compounds with two or more benzene rings whose hydroxylated metabolites (OH-PAHs) are excreted in urine. Human PAH exposure is therefore commonly estimated based on urinary OH-PAH concentrations. However, no study has compared PAH exposure estimates based on urinary OH-PAHs to measurements of PAH levels in blood samples. Estimates of PAH exposure based solely on urinary OH-PAHs may thus be subject to substantial error. To test this hypothesis, paired measurements of parent PAHs in serum and OH-PAHs in urine samples from 480 participants in Guangzhou, a typical developed city in southern China, were used to investigate differences in the estimates of human PAH exposure obtained by sampling different biological matrices. The median PAH concentration in serum was 4.05 ng mL⁻¹, which was lower than that of OH-PAHs in urine (8.33 ng mL⁻¹). However, serum pyrene levels were significantly higher than urinary levels of its metabolite 1-hydroxypyrene. Concentrations of parent PAHs in serum were not significantly correlated with those of their metabolites in urine with the exception of phenanthrene, which exhibited a significant negative correlation. Over 28% of the participants had carcinogenic risk values above the acceptable cancer risk level of 10⁻⁶. Overall, estimated human exposure and health risks based on urinary 1-hydroxypyrene levels were only 13.6% of those based on serum pyrene measurements, indicating that estimates based solely on urine sampling may substantially understate health risks due to PAH exposure.
Show more [+] Less [-]Polycyclic aromatic hydrocarbon contamination along roads based on levels on vehicle window films
2021
Zhang, Weiwei | Su, Penghao | Tomy, Gregg T. | Sun, Dan | Yin, Fang | Chen, Lisu | Ding, Yongsheng | Li, Yifan | Feng, Daolun
Vehicular emissions are known to be major contributors of airborne polycyclic aromatic hydrocarbons (PAHs) in cities. In order to assess the long-term contamination of PAHs along roads, we collected organic films from vehicle windows (26 private cars and 4 buses, in Shanghai, China) and used mathematical models to convert the film-bound PAH concentrations to the airborne PAH concentrations. The field measurements of airborne PAHs revealed that the partitioning and Level III fugacity model was suitable to estimate the airborne concentrations of high and low volatile PAHs (expect for naphthalene), respectively. The total airborne PAH concentrations along roads in Shanghai ranged from 0.83 to 3.37 μg m⁻³ and the incremental lifetime cancer risks (ILCRₜₒₜₐₗ) by exposure to PAHs along roads were greater than the USEPA lower guideline of 10⁻⁶, indicating non-negligible carcinogenic risks to drivers and passengers, especially via ingestion processes. This study provided a practicable method to investigate long-term air contamination of PAHs in vehicles and along roads based on film-bound PAH on vehicle windows. In addition, it was also possible to investigate the health risk in vehicles as a result of exposure to PAHs. Comparisons of PAHs between roads and shipping lanes also facilitated the delineation of vehicular and shipping PAH inventories.A capsule that summarizes the main finding of the work: Investigating film-bound PAH on vehicle windows is a practicable pathway to investigate the long-term contamination of PAHs in vehicles and along roads. This method can not only simplify the sampling processes, but the model calculations. The results also enabled investigations into ILCR in vehicles and specified source apportionment of traffic PAHs.
Show more [+] Less [-]Targeting the right parameters in PAH remediation studies
2021
Davin, Marie | Colinet, Gilles | Fauconnier, Marie-Laure
Contaminated land burdens the economy of many countries and must be dealt with.Researchers have published thousands of documents studying and developing soil and sediment remediation treatments. Amongst the targeted pollutants are the polycyclic aromatic hydrocarbons (PAHs), described as a class of persistent organic compounds, potentially harmful to ecosystems and living organisms.The present paper reviews and discusses three scientific trends that are leading current PAH-contaminated soil/sediment remediation studies and management.First, the choice of compounds that are being studied and targeted in the scientific literature is discussed, and we suggest that the classical 16 US-EPA PAH compounds might no longer be sufficient to meet current environmental challenges.Second, we discuss the choice of experimental material in remediation studies. Using bibliometric measures, we show the lack of PAH remediation trials based on co-contaminated or aged-contaminated material.Finally, the systematic use of the recently validated bioavailability measurement protocol (ISO/TS 16751) in remediation trials is discussed, and we suggest it should be implemented as a tool to improve remediation processes and management strategies.
Show more [+] Less [-]Characterization of polycyclic aromatic compounds in historically contaminated soil by targeted and non-targeted chemical analysis combined with in vitro bioassay
2021
Titaley, Ivan A. | Lam, Monika M. | Bülow, Rebecca | Enell, Anja | Wiberg, Karin | Larsson, Maria
Soil samples from a contaminated site in Sweden were analyzed to identify the presence of 78 polycyclic aromatic compounds (PACs) using gas chromatography coupled with mass spectrometry (GC-MS). The target analysis revealed large contributions not only from polycyclic aromatic hydrocarbons (PAHs), but also from alkylated- and oxygenated-PAHs (alkyl- and oxy-PAHs, respectively), and N-heterocyclics (NPACs). PAC profiles indicated primarily pyrogenic sources, although contribution of petrogenic sources was also observed in one sample as indicated by a high ratio of alkylated naphthalene compared to naphthalene. The aryl hydrocarbon receptor (AhR)-activity of the soil extracts was assessed using the H4IIe-pGudluc 1.1 cells bioassay. When compared with the calculated total AhR-activity of the PACs in the target list, 35–97% of the observed bioassay activity could be explained by 62 PACs with relative potency factors (REPs). The samples were further screened using GC coupled with Orbitrap™ high resolution MS (GC-HRMS) to investigate the presence of other PACs that could potentially contribute to the AhR-activity of the extracts. 114 unique candidate compounds were tentatively identified and divided into four groups based on their AhR-activity and environmental occurrence. Twelve substances satisfied all the criteria, and these compounds are suggested to be included in regular screening in future studies, although their identities were not confirmed by standards in this study. High unexplained bio-TEQ fractions in three of the samples may be explained by tentatively identified compounds (n = 35) with high potential of being toxic. This study demonstrates the benefit of combining targeted and non-targeted chemical analysis with bioassay analysis to assess the diversity and effects of PACs at contaminated sites. The applied prioritization strategy revealed a number of tentatively identified compounds, which likely contributed to the overall bioactivity of the soil extracts.
Show more [+] Less [-]Construction of a regional inventory to characterize polycyclic aromatic hydrocarbon emissions from coal-fired power plants in Anhui, China from 2010 to 2030
2021
Wang, Ruwei | Cai, Jiawei | Cai, Feixuan | Xia, Linlin | Sun, Xiangfei | Zeng, E. Y. (Eddy Y.)
The infrastructures of coal-fired power plants in China have changed significantly since 2010, but the magnitude and characteristics of polycyclic aromatic hydrocarbon (PAH) emissions remain to be updated. In the present study, a unit-based PAH emission inventory for coal-fired power plants between 2010 and 2017 was constructed for Anhui Province, China. Atmospheric PAH emissions from pulverized coal (PC) and circulating fluidized bed (CFB) units in 2017 were 8600 kg and 7800 kg, respectively. The emission rates and intensities for CFB units (7.2 kg ton⁻¹ and 2.1 kg MW⁻¹) were significantly higher than those for PC units (1.1 kg ton⁻¹ and 0.19 kg MW⁻¹), primarily because CFB boilers were operated at lower combustion temperatures and poor combustion conditions compared to PC boilers. The distribution patterns of PAH emissions across different age groups largely reflected the time periods for constructing coal-fired units in Anhui and for the transition of small units to large ones. The accomplishment of ultralow emission technologies and phase-out of outdated coal-fired units were responsible for the decreasing trend of PAH emissions between 2012 and 2017. The warmer summer in 2013 and 2017 and colder winter in 2011 compared to other years probably caused increased use of air conditioners, resulting in increased electricity consumption and PAH emissions. Future PAH emissions would decrease by 45–57% during 2017–2030, benefitting from power plant fleet optimization, i.e., phasing out outdated coal-fired units and replacing them with large ones. With the best available optimized power plant fleets and end-of-pipe control measures accomplished in Anhui’s CFPPs, PAH emissions in 2030 would potentially be reduced by 56–65%.
Show more [+] Less [-]Nitrate-assisted biodegradation of polycyclic aromatic hydrocarbons (PAHs) in the water-level-fluctuation zone of the three Gorges Reservoir, China: Insights from in situ microbial interaction analyses and a microcosmic experiment
2021
Han, Xinkuan | Wang, Fengwen | Zhang, Daijun | Feng, Ding | Zhang, Lilan
An increase in polycyclic aromatic hydrocarbon (PAH) pollution poses significant challenges to human and ecosystem health in the Three Gorges Reservoir (TGR) of the Yangtze River. Based on the combination of PAH analysis with qPCR and high-throughput sequencing of bacteria, 32 topsoil samples collected from 16 sites along the TGR were used to investigate the distribution and biodegradation pathways of PAHs in the water-level-fluctuation zone (WLFZ). The results indicated that the concentrations of PAHs were 43.8–228.2 and 30.8–206.3 ng/g soil (dry weight) under the high- and low-water-level (HWL and LWL) conditions, respectively. The PAH concentration in urban areas was higher than that in rural areas. Under both the HWL and LWL conditions, the abundance of the bamA gene, a biomarker of anaerobic PAH biodegradation, was significantly higher than that of the ring-hydroxylating-dioxygenase (RHD) gene, a biomarker of aerobic PAH biodegradation. The abundance of the bamA gene was significantly positively correlated with PAHs (R² = 0.8), and the biodegradation percentage of PAHs incubated anaerobically was greater than that in the aerobically incubated microcosm experiments. These data implicated a key role of the anaerobic pathway in PAH biodegradation. Co-occurrence network analysis suggested that anaerobic Anaerolineaceae, Dechloromonas, Bacteroidetes_vadin HA17 and Geobacter were key participants in the biodegradation of PAHs. The diversity analysis of functional bacteria based on the bamA gene and microcosm experiments further demonstrated that nitrate was the primary electron acceptor for PAH biodegradation. These findings provide a new perspective on the mechanism of PAH biodegradation in the TGR and knowledge that can be used to develop strategies for environmental management.
Show more [+] Less [-]Contamination and human health risks of polycyclic aromatic hydrocarbons in surface soils from Tianjin coastal new region, China
2021
Shi, Rongguang | Li, Xiaohua | Yang, Yanying | Fan, Ying | Zhao, Zongshan
Polycyclic aromatic hydrocarbons (PAHs) in urban soils are of increasing concern because of their potential toxicity and persistence. However, there is limited information about PAHs in Tianjin coastal new region, although it is an important economic and industrial center in Northern China. Here we determined the concentrations of PAHs in 210 surface soil samples collected from this region according to administrative divisions covering Han’gu district, Tanggu district, and Dagang district, to evaluate their contamination and potential cancer risks. The concentrations of 16 PAHs ranged from 58.2 to 9160 ng g⁻¹, and the highest concentration was found in Han’gu district. According to the incremental lifetime cancer risk (ILCR) model, the soils from Han’gu district and Dagang district posed a moderate carcinogenic risk to residents, and dermal contact was the main exposure pathway. Besides, ILCRs for children through ingestion were comparable to those for adults but apparently higher than adolescents, while ILCRs of dermal contact for adults were higher than children and adolescents. Comparisons between the layout of industrial zones and the distributions of PAHs as well as ILCRs indicate that PAHs accumulating in soils and then incurring risk areas is partly controlled by the economic and industrial structure.
Show more [+] Less [-]Co-pyrolysis of food waste and wood bark to produce hydrogen with minimizing pollutant emissions
2021
In this study, the co-pyrolysis of food waste with lignocellulosic biomass (wood bark) in a continuous-flow pyrolysis reactor was considered as an effective strategy for the clean disposal and value-added utilization of the biowaste. To achieve this aim, the effects of major co-pyrolysis parameters such as pyrolysis temperature, the flow rate of the pyrolysis medium (nitrogen (N₂) gas), and the blending ratio of food waste/wood bark on the yields, compositions, and properties of three-phase pyrolytic products (i.e., non-condensable gases, condensable compounds, and char) were investigated. The temperature and the food waste/wood bark ratio were found to affect the pyrolytic product yields, while the N₂ flow rate did not. More non-condensable gases and less char were produced at higher temperatures. For example, as the temperature was increased from 300 °C to 700 °C, the yield of non-condensable gases increased from 6.3 to 17.5 wt%, while the yield of char decreased from 63.6 to 30.6 wt% for the co-pyrolysis of food waste and wood bark at a weight ratio of 1:1. Both the highest yield of hydrogen (H₂) gas and the most significant suppression of the formation of phenolic and polycyclic aromatic hydrocarbon (PAH) compounds were achieved with a combination of food waste and wood bark at a weight ratio of 1:1 at 700 °C. The results suggest that the synergetic effect of food waste and lignocellulosic biomass during co-pyrolysis can be exploited to increase the H₂ yield while limiting the formation of phenolic compounds and PAH derivatives. This study has also proven the effectiveness of co-pyrolysis as a process for the valorization of biowaste that is produced by agriculture, forestry, and the food industry, while reducing the formation of harmful chemicals.
Show more [+] Less [-]In-depth investigation of Sodium percarbonate as oxidant of PAHs from soil contaminated with diesel oil
2021
Cavalcanti, Jorge Vinicius Fernandes Lima | Fraga, Tiago José Marques | Loureiro Leite, Mirella de Andrade | dos Santos e Silva, Daniella Fartes | de Lima, Valmir Félix | Schuler, Alexandre Ricardo Pereira | do Nascimento, Clístenes Williams Araújo | da Motta Sobrinho, Maurício Alves
Sodium percarbonate (SPC, 2Na₂CO₃∙3H₂O₂), is a compound that can be used under multiple environmental applications. In this work, SPC was employed as oxidant in the treatment of soil contaminated with diesel oil. The soil samples were collected during the earthmoving stage of RNEST Oil Refinery (Petrobras), Brazil. Then, the samples were air-dried, mixed and characterized. Subsequently, raw soil was contaminated with diesel and treated by photo-Fenton reaction (H₂O₂/Fe²⁺/UV). SPC played a significant role in the generation of hydroxyl radicals under the catalytic effect of ferrous ions (Fe²⁺), hydrogen peroxide (H₂O₂) and radiation. These radicals provoked the photodegradation of polycyclic aromatic hydrocarbons (PAHs), in the soil remediation. A factorial design 3³ was carried out to assess the variables which most influenced the decrease in total organic carbon (TOC). The study was performed with the following variables: initial concentration of [H₂O₂] and [Fe²⁺], between 190.0 and 950.0 mmol L⁻¹ and 0.0–14.4 mmol L⁻¹, respectively. UV radiation was supplied from sunlight, blacklight lamps, and system without radiation. All experiments were performed with 5.0 g of contaminated soil in 50.0 mL of solution. The initial concentration of Fe²⁺ showed the statistically most significant effect. The oxidation efficiency evaluated in the best condition showed a decrease from 34,765 mg kg⁻¹ to 15,801 mg kg⁻¹ in TOC and from 85.750 mg kg⁻¹ to 20.770 mg kg⁻¹ in PAHs content. Moreover, the sums of low and high molecular weight polycyclic aromatic hydrocarbons (LMW-PAHs and HMW-PAHs) were 19.537 mg kg⁻¹ and 1.233 mg kg⁻¹, respectively. Both values are within the limits recommended by the United Sates Environmental Protection Agency (USEPA) and evidenced the satisfactory removal of PAHs from contaminated soil, being an alternative to classic oxidation protocols.
Show more [+] Less [-]Biomonitoring of polycyclic aromatic hydrocarbons in the urine of lactating mothers: Urinary levels, association with lifestyle factors, and risk assessment
2021
F. Fernández, Sandra | Pardo, Olga | Pastor, Agustín | Yusà, Vicent | Vento, M. | Cernada, M. | Gormaz, M. | Kuligowski, J. | Sánchez, A. | Torres, E. | Correcher, P. | Núñez, A. | Parra, A. | Ramón, A.
Polycyclic aromatic hydrocarbons (PAHs) are pollutants produced during incomplete combustion of organic matter and several industrial processes. Humans can be exposed to PAHs through ingestion of food, inhalation of tobacco smoke or polluted air, and dermal contact, causing immunologic, developmental, and reproductive problems.In the present research, eleven metabolites of PAHs were analyzed in the urine of 110 lactating women living in Spain (2015). PAH metabolites were extracted from the urine samples by liquid-liquid extraction and their determination was performed by liquid chromatography coupled to tandem mass spectrometry. In addition, information on lifestyle and dietary habits of the participants was collected using a questionnaire.All the PAH metabolites were detected in more than 70% of the samples, except for 3-hydroxybenzo(a)pyrene which was detected in less than 1% of the samples. The highest urinary levels were found for naphthalene metabolites, with geometric means of 0.8 (1-hydroxynaphthalene) and 7.1 ng ml⁻¹ (2-hydroxynaphthalene). The statistical analysis showed that smoking status, as well as the ingestion of certain food groups (vegetables, cereals, oils and fats, smoked fish and coffee), were the main influencing factors of exposure to PAHs.The estimated daily intake (EDI) was calculated for naphthalene, fluorene, phenanthrene, and pyrene, ranging from 6 to 1522 ng kg⁻¹·day⁻¹. The non-cancer risk associated to PAH exposure was estimated, showing hazard quotients (HQs) and hazard indexes (HIs) below 1. Therefore, it did not reveal a significant health risk for Spanish women due to PAH exposure.
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