Fine particulate matter (PM2.5) is a significant health issue in Chinese megacities. However, little information is available regarding the PM2.5-bound toxic organics, especially their sources, atmospheric transformations, and health implications. In this study, we assessed the levels of polycyclic aromatic hydrocarbons (PAHs) and their nitrated, hydroxylated, and oxygenated derivatives (i.e., NPAHs, OHPAHs, and OPAHs, respectively) in PM2.5 collected in Beijing over a one-year period. The median concentration of 23 PAHs, 15 NPAHs, 16 OHPAHs, and 7 OPAHs in PM2.5 was 53.8, 1.14, 1.40, and 3.62 ng m−3, respectively. Much higher concentrations and mass percentages for all species were observed in the heating season, indicating a higher toxicity of PM2.5 during this period of time. Positive matrix factorization (PMF) was applied to apportion the sources of PAHs and their derivatives. It was found that traffic emissions in the non-heating season, and coal combustion and biomass burning in the heating season, were the major primary sources of PAHs and their derivatives. Secondary formation, however, contributed significantly to the derivatives of PAHs (especially NPAHs and OPAHs) in the non-heating season, suggesting significant impacts of atmospheric transformation on the toxicity of PM2.5.

https://agupubs.onlinelibrary.wiley.com/doi/pdf/10.1002/2015JD023628

Sources, transformation, and health implications of PAHs and their nitrated, hydroxylated, and oxygenated derivatives in PM2.5 in Beijing

Selection of oxidant doses for in situ chemical oxidation of soils contaminated by polycyclic aromatic hydrocarbons (PAHs): A review.

Multiple organ injury in male C57BL/6J mice exposed to ambient particulate matter in a real-ambient PM exposure system in Shijiazhuang, China.

Airborne particulate matter (PM) has been collected at four cities in Japan starting in the late 1990s, at five or more major cities in China, Korea and Russia starting in 2001 and at the Noto Peninsula starting in 2004. 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 were in the order, China>Russia≫Korea=Japan, with seasonal change (winter>summer). During the observation period, concentrations of PAHs and NPAHs in Japanese cities significantly decreased but the increases in the PAH concentration were observed in Chinese and Russian cities. Concentrations of PAHs and NPAHs were higher in the Northern China than those in the Southern China. At 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 were high in winter and low in summer every year. A cluster analysis and back trajectory analysis indicated that PAHs and NPAHs were long-range transported from Northeastern China, where coal burning systems such as coal-heating boilers are considered to be the major contributors of PAHs and NPAHs. A dramatic change in atmospheric concentrations of PAHs and NPAHs in East Asia suggests the rapid and large change of PM2.5 pollution in East Asia. Considering the adverse health effects of PM2.5, continuous monitoring of atmospheric PAHs and NPAHs is necessary in this area.

Environmental Behaviors and Toxicities of Polycyclic Aromatic Hydrocarbons and Nitropolycyclic Aromatic Hydrocarbons.

The heterogeneous reactions of ambient particulate matter (PM)-bound polycyclic aromatic hydrocarbons (PAHs) and nitro-PAHs (NPAHs) with NO3/N2O5, OH radicals, and O3 were studied in a laboratory photochemical chamber. Ambient PM2.5 and PM10 samples were collected from Beijing, China, and Riverside, California, and exposed under simulated atmospheric long-range transport conditions for O3 and OH and NO3 radicals. Changes in the masses of 23 PAHs and 20 NPAHs, as well as the direct and indirect-acting mutagenicity of the PM (determined using the Salmonella mutagenicity assay with TA98 strain), were measured prior to and after exposure to NO3/N2O5, OH radicals, and O3. In general, O3 exposure resulted in the highest relative degradation of PM-bound PAHs with more than four rings (benzo[a]pyrene was degraded equally well by O3 and NO3/N2O5). However, NPAHs were most effectively formed during the Beijing PM exposure to NO3/N2O5. In ambient air, 2-nitrofluoranthene (2-NF) is formed from the gas-phase NO3 radical- and OH radical-initiated reactions of fluoranthene, and 2-nitropyrene (2-NP) is formed from the gas-phase OH radical-initiated reaction of pyrene. There was no formation of 2-NF or 2-NP in any of the heterogeneous exposures, suggesting that gas-phase formation of NPAHs did not play an important role during chamber exposures. Exposure of Beijing PM to NO3/N2O5 resulted in an increase in direct-acting mutagenic activity which was associated with the formation of mutagenic NPAHs. No NPAH formation was observed in any of the exposures of the Riverside PM. This was likely due to the accumulation of atmospheric degradation products from gas-phase reactions of volatile species onto the surface of PM collected in Riverside prior to exposure in the chamber, thus decreasing the availability of PAHs for reaction.

/pdf/heterogeneous-reactions-of-particulate-matter-bound-pahs-and-4xhiby6moe.pdf

Heterogeneous Reactions of Particulate Matter-Bound PAHs and NPAHs with NO3/N2O5, OH Radicals, and O3 under Simulated Long-Range Atmospheric Transport Conditions: Reactivity and Mutagenicity

Particulates exhausted from two types of diesel engines (DEPs), burning-derived particulates from three types of coal (CBPs) and burning-derived particulates from three types of wood (WBPs) were separated into four fractions by silica-gel column chromatography using n -hexane, n -hexane–dichloromethane (3:1, v/v), dichloromethane and methanol, as the corresponding eluents. The indirect-acting mutagenicity of each fraction was assayed by the Ames test using the Salmonella typhimurium TA100 strain with S9 mix and the direct-acting mutagenicity was assayed using the S. typhimurium TA98 strain without S9 mix. The polycyclic aromatic hydrocarbons (PAHs) and nitropolycyclic aromatic hydrocarbons (NPAHs) of each fraction were determined by high-performance liquid chromatography (HPLC). Both direct- and indirect-acting of mutagenicities were the highest in samples of DEPs. The contributions of PAHs in samples of WBPs and NPAHs in DEPs were the largest, respectively.

Indirect- and direct-acting mutagenicity of diesel, coal and wood burning-derived particulates and contribution of polycyclic aromatic hydrocarbons and nitropolycyclic aromatic hydrocarbons.

Long-range transport of fluoride in East Asia monitored at Noto Peninsula, Japan.

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Indirect- and direct-acting mutagenicity of diesel, coal and wood burning-derived particulates and contribution of polycyclic aromatic hydrocarbons and nitropolycyclic aromatic hydrocarbons.

Long-range transport of fluoride in East Asia monitored at Noto Peninsula, Japan.