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Abstract Nitrotriphenylenes (NTPs), which include the highly mutagenic isomer 2-nitrotriphenylene (2-NTP), have been detected in airborne particles. From a public hygienic point of view, it is necessary to study the environmental occurrence of NTPs in detail. In this study, concentrations of five nitrated polycyclic aromatic hydrocarbons (nitro-PAHs) including NTPs in airborne particles and of nitrogen oxides (NOx; NO+NO2) and carbon monoxide (CO), at a location in South Osaka, Japan, were measured at 3 h intervals. It was found that the diurnal variations in the concentrations of 1-nitropyrene (1-NP), NOx, and CO were similar, being high early in the morning and late in the evening. This finding indicates that the occurrence of 1-NP is affected significantly by primary emissions, particularly by automotive emissions. The concentration change in 1-nitrotriphenylene was similar to that of 2-nitropyrene produced by an atmospheric OH radicalinitiated reaction. On the contrary, the variations in the concentrations of 2-nitrofluoranthene (2-NF) and 2-NTP were significantly different from those of the other nitro-PAHs, i.e., their concentrations increased during the nighttime, suggesting that neither 2-NF nor 2-NTP was emitted from the primary sources, but were formed via the NO3 radicalinitiated nitration of the parent fluoranthene and triphenylene (TP) in the atmosphere. Based on the ambient concentration of 2-NTP and the reported rate constant for the reaction of TP with NO3 radicals, the yield of 2-NTP from the gas-phase NO3 radical-initiated reaction of TP was estimated to be 23%.

PM2.1 was collected at urban and suburban elementary schools in Shanghai during two sampling periods in cold and warm seasons in 2007. Nine polycyclic aromatic hydrocarbons (PAHs) and ten nitro-polycyclic aromatic hydrocarbons (NPAHs) in PM2.1 were determined. During both seasons, the concentrations of PAHs and NPAHs at urban and suburban schools were not significantly different (p>0.05) and were higher in the cold period than in the warm period. According to the diagnostic ratios, PAHs and NPAHs at both schools were subject to the mixed effects of vehicle emission and coal combustion during both periods. Moreover, the results of the backward trajectory showed that PAHs and NPAHs were more susceptible to external polluted air masses in the cold period. At both urban and suburban schools, the inhalation cancer risk of PAHs and NPAHs in PM2.1 for children during elementary period was dozens of times of the acceptable risk level regulated by the U.S.EPA, highlighting the adverse impact of exposure to PAHs and NPAHs on the healthy development of children.

Although polycyclic aromatic hydrocarbons (PAHs) are toxic, the effects of oxidized PAHs on health and biological responses remain unclear. In this study, we examined the in vitro effects of varying concentrations of pyrene, a type of PAH, and its quinone forms, namely 4,5-pyrenequinone (PyQ) and 1,8-PyQ + 1,6-PyQ, on human lung epithelial (BEAS-2B) cells. We evaluated cell viability, apoptosis, and the production of interleukin (IL)-6, IL-8, soluble intercellular adhesion molecule-1 (sICAM-1), and reactive oxygen species (ROS). Exposure to 1 μM 4,5-PyQ or 1,8-PyQ + 1,6-PyQ increased the cellular activity. At 3 µM, 4,5-PyQ increased the number of late apoptotic and/or necrotic cells compared with those in the control, whereas 1,8-PyQ + 1,6-PyQ increased the number of dead cells. Exposure to 4,5-PyQ at 10 µM decreased IL-6 production and exposure to both 4,5-PyQ and 1,8-PyQ + 1,6-PyQ at 3 or 10 µM decreased IL-8 production. sICAM-1 production was increased after 1,8-PyQ + 1,6-PyQ exposure at 10 µM. In the presence of cells, 4,5-PyQ and 1,8-PyQ + 1,6-PyQ increased ROS production significantly in a concentration-dependent manner; similar results were observed with 1,8-PyQ + 1,6-PyQ without cells. Overall, our results suggest that oxidized PAHs induce stronger respiratory toxicity/inflammatory responses than PAHs.

Atmospheric particulate matter (PM) contains various chemicals, some of which generate in vivo reactive oxygen species (ROS). Owing to their high reactivity and oxidation ability, ROS can cause various diseases. To understand how atmospheric PM affects human health, we must clarify the PM components having oxidative potential (OP) leading to ROS production. According to previous studies, OP is exhibited by humic-like substances (HULIS) in atmospheric PM. However, the OP-dependence of the chemical structures of HULIS has not been clarified. Therefore, in this study, humic acid (HA, a model HULIS material) was exposed to ozone and ultraviolet (UV) irradiation, and its OP and structures were evaluated before and after the reactions using dithiothreitol (DTT) assay and Fourier transform infrared (FT-IR), respectively. The OP of HA was more significantly increased by UV irradiation than by ozone exposure. FT-IR analysis showed an increased intensity of the C=O peak in the HA structure after UV irradiation, suggesting that the OP of HA was increased by a chemical change to a more quinone-like structure after irradiation.

1-Nitropyrene (1-NP), 2-NP and 2-nitrofluoranthene (2-NFR) are useful markers for studying the atmospheric behaviors of polycyclic aromatic hydrocarbons (PAHs) and nitropolycyclic aromatic hydrocarbons (NPAHs). However, present methods for measuring trace levels of these compounds are less-sensitive and laborious. Here we describe several improvements to a previously reported high-performance liquid chromatography-chemiluminescence detection system that allows it to determine trace levels of 1-, 2-NPs and 2-NFR. The proposed system was equipped with a reducer column packed with Pt/Rh instead of zinc whose life-time was limited. The combination of Cosmosil MS-II (monomeric ODS) and AR-II (polymeric ODS) columns was used instead of polymeric ODS columns as the separator column to improve the separation. An ethanol mixture with acetate buffer (pH 5.5) was used in place of an acetonitrile mixture with the same buffer to activate the reducer column. The same ethanol mixture was used as the mobile phase for the clean-up column. The switching time of the column switching valve was optimized to concentrate the amino-derivatives of above NPAHs quantitatively on the concentrator column. The concentrations of bis(2,4,6-trichlorophenly) oxalate and hydrogen peroxide in the chemiluminescence reagent solution were optimized to 0.4 mM and 30 mM, respectively, to increase the sensitivity. Under the above conditions, the detection limits (S/N=3) of 1-, 2-NPs and 2-NFR were 1 fmol (0.25 pg), 10 fmol (2.5 pg) and 4 fmol (1 pg), respectively. The proposed system was effectively used to determine trace levels of 1-, 2-NPs and 2-NFR in airborne particulates collected at Noto Peninsula. The atmospheric concentrations of 1-, 2-NPs and 2-NFR were not more than sub pg m-3 levels. They were higher in winter (January) than in summer (July). In both seasons, the concentrations were in decreasing order, [2-NFR]>[1-NP]>[2-NP].

Airborne particulates were collected in three different size fractions (>7 μm; 2.1-7 μm;

Hazardous polycyclic aromatic hydrocarbons (PAHs) and nitropolycyclic aromatic hydrocarbons (NPAHs) are mainly originated from imperfect combustion of fossil fuels such as petroleum and coal. The consumptions of not only petroleum but also coal have been increasing in the East Asian countries. This review describes the result of international collaboration research concerning characteristics and major contributors of atmospheric PAHs and NPAHs in cities in Japan, Korea, China and Russia. We collected airborne particulates in ten cities in the above countries and six PAHs and eleven NPAHs were determined by HPLC methods using fluorescence and chemiluminescence detections. The total PAH concentrations were much higher in Chinese cities (Fushun, Tieling, Shenyang and Beijing) than those in other cities (Vladivostok, Busan, Kanazawa, Kitakyushu, Sapporo and Tokyo). The total NPAH concentrations were also higher in Chinese cities than those in the other cities. The [NPAH]/[corresponding PAH] ratios are much larger in diesel-engine exhaust particulates than those in coal-burning particulates. The [1-nitropyrene]/[pyrene] ratio of airborne particulates was much smaller in the four Chinese cities, suggesting that coal combustion systems such as coal heaters were the main contributors. On the other hand, the ratios were larger in Korean and Japanese cities, suggesting the large contribution of diesel-engine vehicles.

Airborne particulates have been continuously collected at four cities in Japan starting in the late 1990s, at major cities in China, Korea and Russia starting in 2001 and at Noto peninsula starting in 2004. After extracting and cleaning up particulates, nine polycyclic aromatic hydrocarbons (PAHs) and eleven nitropolycyclic aromatic hydrocarbons (NPAHs) were determined by HPLC with fluorescence and chemiluminescence detections, respectively. Annual concentrations of PAHs and NPAHs at the cities were in the order, China>Russia>Korea>Japan. Concentrations of PAHs and NPAHs in Japanese cities signi fcantly decreased but different tendencies were observed in Chinese and Russian cities. On the Noto peninsula, which is in the main path of winter northwest winds and a year-round jet stream that blow from the Asian continent to Japan, the concentrations of PAHs and NPAHs were high in winter and low in summer every year. A cluster analysis and back trajectory analysis indicated that PAHs and NPAHs at the Noto peninsula in winter mainly came from coal burning systems in Northeast China. [ABSTRACT FROM AUTHOR]

Diesel exhaust particles (DEPs) contain oxygen-containing polycyclic aromatic hydrocarbons (PAHs) called quinoid PAHs. Some quinoid PAHs generate free radicals as they undergo enzymatic and nonenzymatic redox cycling with their corresponding semiquinone radicals. Reactive oxygen species (ROS) produced by these reactions can cause severe oxidative stress connected with inflammatory processing. Although humans and animals are continuously exposed to these chemicals in the environment, little is known about which quinoid PAHs are active. In this study, we estimated the intracellular ROS production and nuclear factor kappa B (NF-κB) translocation in A549 cells exposed to isomers of quinoid PAHs having two to four rings. We found that both acenaphthenequinone (AcQ) and 9,10-phenanthrenequinone (PQ) enhanced ROS generation and that AcQ translocated NF-κB from the cytosol to the nucleus. However, PQ, which has been reported to induce apoptosis, did not influence NF-κB activation. In addition, AcQ induced cyclooxygenase-2 (COX-2) expression which is a key enzyme in the inflammatory processing involved in the activation of NF-κB. Upregulation of NF-κB and COX-2 expression by AcQ treatment was suppressed by the antioxidant N-acetylcysteine (NAC). These results provide that AcQ might play an important role in human lung inflammatory diseases as an air pollutant. [ABSTRACT FROM AUTHOR]

Quinoid polycyclic aromatic hydrocarbons are potent redox-active compounds that undergo enzymatic and nonenzymatic redox cycling with their semiquinone radical. We previously reported that acenaphthenequinone (AcQ) can damage human lung epithelial A549 cells through the formation of reactive species (RS). However, the biochemical mechanisms by which RS-generating enzymes cause oxidative burst during AcQ exposure remain elusive. Here we examined the biochemical mechanism of AcQ-induced RS generation by using selective metabolic inhibitors in A549 cells. We found that AA861, a 5-lipoxygenase (5-LO)–specific inhibitor significantly decreases RS generation. This inhibition of RS seems to be 5-LO specific because other inhibitors did not suppress AcQ-induced RS generation by nicotinamide adenine nucleotide phosphate (reduced) oxidase and/or xanthine oxidase. In addition, the inhibition of 5-LO by AA861 markedly reduced AcQ-induced nuclear factor kappa B (NF-κB) activation. We further found the activation of 5-LO pathway by exposing cells to AcQ mediates the secretion of inflammatory leukotriene B4, which can be significantly suppressed by a potent RS scavenger, N-acetylcysteine. Thus, based on our findings, we propose that AcQ-induced damage is likely due to increased RS generation and NF-κB activity through 5-LO activation. [ABSTRACT FROM AUTHOR]

Particulate air pollutants and mineral fibers activate inflammatory cells to release oxidants, which contribute to inflammation and injury in the lower respiratory tract. Our aim was to compare the role of silica particle size with mineral fiber length and width in the ability to induce superoxide release from rat alveolar macrophages. We estimated the ability of four types of silica particle samples, with different mode diameter, and three types of mineral fiber samples, with different geometric mean lengths and widths, to induce lucigenin-dependent chemiluminescence (CL) from the cells per number of dust particles (i.e., silica particles and mineral fibers). A close positive correlation was observed between dust size and the ability to induce CL in silica as well as mineral fiber samples. Moreover, the ability of silica samples to induce CL was weaker than that of long mineral fiber sample. This ability increased at a larger rate in small silica particle and thin mineral fiber samples than in large silica particle and thick mineral fiber samples at the initial stage of administration. These results suggest that the kinetics of the induction superoxide release from macrophages is similar between silica particles and mineral fibers; moreover, this depends on silica particle size and mineral fiber geometry. Finally, large silica particles were more active than small ones. [ABSTRACT FROM AUTHOR]

A comparative study of polycyclic aromatic hydrocarbons (PAHs) associated with particulate matter (TSP) in the ambient air in an urban area in Ho Chi Minh City, Vietnam and in Osaka, Japan was carried out from 2005 to 2006. The objective of this study was to investigate the environmental levels, emission sources, seasonal variations and health risk of eleven PAHs in the two cities, especially Ho Chi Minh City where air pollution is becoming a serious concern. The results showed that the concentrations of TSP and total PAHs were significantly higher in Ho Chi Minh City than levels in Osaka. The concentrations of 5-and 6-ring PAHs (BeP, BbF, BkF, BaP, BghiP and InP) were much higher in TSP samples in Ho Chi Minh City than in Osaka, accounting for 82% and 51% of total PAHs, respectively. These PAHs are known to be highly carcinogenic and mutagenic in humans. Vehicular emission is suggested as one of the main pollution sources of PAHs in both cities. Motorcycles and gasoline automobiles are suggested as the main emission sources of PAHs in Ho Chi Minh City, whereas diesel automobiles are the primary source in Osaka. Seasonal variations of PAHs were observed in this study; higher concentrations of PAHs were found in the rainy season (May–December) and lower concentrations corresponded to the dry season (February–April) in Ho Chi Minh City, while higher concentrations of PAHs were observed in the winter (November–January) in Osaka. The number of sunshine hours was an important meteorological factor affecting seasonal variations of PAHs in Ho Chi Minh City, while the temperature was a main factor causing the variations of PAHs in Osaka. The high BaP equivalent concentration of 5-and 6-ring PAHs even in the ambient air is an alarming signal for harmfulness to human health and environmental quality in Ho Chi Minh City. [Copyright &y& Elsevier]