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Some Polycyclic Aromatic Compounds (PACs) such as nitrated-PAHs (NPAHs), oxygenated-PAHs (OPAHs) and methyl-PAHs (MPAHs) have attracted significant concern due to derivatives have greater potential to be more toxic at low environmental concentrations compared to their PPAHs, particularly in petrochemical industrial region and its surrounding areas surface soils in China. Hence, this article provides an insight into the fate, sources, impacts, and relevance to the external environment of PAH-derivatives based on important emissions source. Moreover, prospective health risk due to their exposure has also been discussed. In this study, the concentration (10 -3  ng/g) of Ʃ18PPAHs, Ʃ11MPAHs, Ʃ12NPAHs, and Ʃ4OPAHs in the park were 9.67 ± 1.40, 3.24 ± 0.54, 0.03 ± 0.02 and 0.19 ± 0.65, respectively, which were 4.47, 3.89, 2.04 and 1.17 times than of them surrounding the region. A decreasing trend of the low molecular weight (2-4Rings) contribution to the total amount of PAHs, while the fraction of high molecular weight (5-6Rings) species showed the opposite trend. According to the principal component analysis (PCA) and diagnostic ratios indicated PAHs in the soil samples have mixed sources from industrial activities, solid fuel combustion, and heavy traffic. Despite the high concentrations of MPAHs and OPAHs, the toxicity equivalency quotients (TEQs) of them were not calculated due to the lack of toxic equivalent factors (TEF), thus current studies on PAH and derivatives could have underestimated their exposure risks. The quality and sustainable management of soils are crucial for human health and sustainable development, while there is lack of public awareness of the severe issue of soil pollution. It is recommended to conduct more intensive monitoring and regional assessments in the future., (© 2024. The Author(s), under exclusive licence to Springer Nature B.V.)

The rapid growth of maritime traffic, transportation, and fishery activities has increased shipping emissions and degraded the air quality in coastal areas. As a result, controlling ocean-based pollution sources have become increasingly important. This study investigated the real-world emission characteristics of oxygenated polycyclic aromatic hydrocarbons (OPAHs, a group of highly toxic semi-volatile organic compounds) from five types of offshore ships using diesel oil: small and medium fishing ships, tug boats, ferry, and engineering ships, under various driving mode. Both gaseous and particle emission factors (EF) of four specific OPAHs were determined in our study. Among the OPAHs species emitted from ships, 9-fluorenone (9FO; 72%) and anthrathrace-9,10-quinone (ATQ; 25%) were the most abundant. The arithmetic mean of the sum of gaseous OPAHs EFs for all ships in this study was 2.5 ± 4.4 mg/kg fuel burned, and the mean particulate OPAHs EF was 4.7 ± 7.9 mg/kg. Small fishing ships had the highest total OPAHs EFs (31.0 ± 17.0 mg/kg). Apart from small fishing ships, there was no significant difference in the total EF of OPAHs for the other four types of ships. The emissions of the four OPAHs are predominantly in the particulate phase. There were no significant differences in the emissions of the four OPAHs under different driving mode. According to estimates, the annual OPAH emissions from the four types of ships in Hainan in 2017 were approximately 4.2 (range: 2.7-7.0) tons, dwarfing the OPAH emissions from diesel-powered on-road vehicles in China (23.5 kg)., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2023 Elsevier Ltd. All rights reserved.)

The current study features PAHs exposure on Karakoram Highway, a route of utmost importance in Pakistan. The drivers of heavy traffic vehicles (HTV) on Karakoram Highway spend long hours amid dense traffic and therefore, inevitably inhale huge amount of PAH carcinogens. The urinary metabolites of PAHs in such drivers (meeting selection criteria n = 48) and a control group (n = 49) were comparatively profiled. The higher urinary biomarkers among ninety-six percent HTV drivers were evident of PAHs exposure. We observed elevated concentrations of urinary benzo[a]pyrene metabolites (3-OH-BaP = 3.53 ± 0.62 ng g -1 creatinine and 9-OH-BaP = 3.69 ± 0.74 ng g -1 creatinine) in HTV driver's samples compared to controls (0.85 ± 0.08 and 0.31 ± 0.03 ng g -1 creatinine, respectively). Interestingly, urinary benzo[a]pyrene metabolites were detected in almost similar amount among HTV drivers irrespective of their working hours. A distinct smoking effect was manifested with rising urinary levels of 1-hydroxypyrene, 2-hydroxyphenanthrene, and 3-hydroxybenzo[a]pyrene with corresponding increase in driving hours per day. These metabolites exhibited characteristic exposures to low molecular weight volatile PAHs that are commonly found in vehicular exhaust. The elevated PAH body burden was directly linked to the nature of their job and the route-long environmental pollution on Karakoram Highway. Additionally, the poor economic status and smoking also increased HTV driver's health vulnerability and significantly declined their health capacity. There was conclusive evidence that HTV drivers were exposed to PAHs during a ride on Karakoram Highway, back and forth, an aspect not reported earlier., (© 2022. The Author(s), under exclusive licence to Springer Nature B.V.)

The deposition of polycyclic aromatic hydrocarbon (PAHs) has far-reaching impacts on Earth's surface system and human health. However, a comprehensive understanding of PAHs' deposition in a high urbanized area is still lacking because of limited field measurements data and rough resolution of current models. In this research, a deposition map of PAHs with a resolution of 2 × 2 km in megacity Shanghai, China was established. Gridded annual total deposition of PAHs from July 2020 to June 2021 ranged from 385 to 10,631 ng/(m 2 ·d), with a mean value of 2,611 ng/(m 2 ·d). The highest PAHs deposition was found over the downtown Shanghai, which received 4.3 times the deposition flux of outlying areas. About 77 % of area in Shanghai was dominated by wet deposition which accounted for 62 % of total deposition in Shanghai. The total deposition showed a trend of summer>fall>spring>winter, which was similar to that of the amount of rain. Source apportionment and geographically weighted regression analysis showed that built-up land and human activities are key driving factors of PAHs' deposition in Shanghai. Our results suggest that intensive human activities could alter the PAHs deposition distribution in Shanghai, and improve the understanding of PAHs' environmental behavior in high urbanized area., Competing Interests: Declaration of Competing Interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2022 Elsevier B.V. All rights reserved.)

Substituted polycyclic aromatic hydrocarbons (SPAHs) have shown higher health and ecological risks than the corresponding parent PAHs (PPAHs) from laboratory studies, their variations in freshwater system, especially in surface sediment and pore water, remain inadequate understanding. In this study, we revealed the coexistence, ecological risk, and multiple factors affecting variations and sources of PPAHs and SPAHs (nitrated PAHs (NPAHs), oxygenated PAHs (OPAHs)) in the surface sediment-pore water system from a typical urban river in Northern China. The concentration ranges of Σ 26 PPAHs, Σ 10 NPAHs, and Σ 4 OPAHs in the surface sediments were 153.0-5367.4, not detected (N.D.)-105.4, and 42.2-1177.0 ng·g -1 dry weight, and fell within 0.6-38.8, N.D.-297.9, and N.D.-212.6 ng·mL -1 in the pore waters. The t-distributed stochastic neighbor embedding (SNE) coupled with the partitioning around medoids (PAM) elucidated spatiotemporal the variations in PAHs, emphasizing the impacts of industrial activities and sewage discharges. Besides the geochemical and hydrochemical conditions, SPAHs were affected by the potential secondary formation, especially during the wet season. The method comparisons indicated the advantages of principal component analysis-multivariate linear regression (PCA-MLR) and n-alkanes model on source identification. PAHs mainly originated from fossil fuel combustion and vehicular exhaust. The top risk quotient (RQ) values for PAHs occurred in the urban and industrial sections. A majority of the surface sediment samples emerged with low to moderate exposure risks, while all the pore water samples showed high exposure risks. The RQs of OPAHs were significantly higher (p < 0.01) than those of PPAHs. The results suggested the secondary formation of SPAHs as an important role in ecological risks of PAHs in the urban river system., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2022 Elsevier B.V. All rights reserved.)

Polycyclic aromatic hydrocarbons (PAHs) derivatives such as oxygenated PAHs (oPAHs) and nitrated PAHs (nPAHs), are receiving raising concerns due to their high toxic potential. Incomplete solid fuel combustion can release large quantities of PAHs derivatives, especially in low-efficiency domestic stoves. In this study, field measurements were conducted in rural Chinese homes to determine emissions of nPAHs and oPAHs from solid fuel combustion. A total of 12 fuel-stove combinations including cooking and space heating activities were investigated. Emission factors (EFs) of total nPAHs and oPAHs were in the range of 1.0-682.1 μg/kg and 0.01-131.7 mg/kg, respectively, with arithmetic means and stand deviations of 53.5 ± 72.5 μg/kg and 13.9 ± 24.4 mg/kg, respectively. The EFs of nPAHs and oPAHs for coal combustion (including honeycomb briquette, coal chunk, and peat tested in this study) were 30.2 ± 28.1 μg/kg and 1.5 ± 2.9 mg/kg, respectively, much lower than that for biomass burning (p < 0.05). The combustion phase could significantly affect the PAHs derivative emissions with higher emissions at initial phase than that at stable phase. Fuel type was found to affect the EFs, composition profiles, and ratios of PAHs derivatives to parent PAHs. This study tries to have an insight of PAHs derivative emissions from various solid fuel combustion, which would be useful in understanding the atmospheric PAHs derivative pollutions in China., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2022 Elsevier B.V. All rights reserved.)

Indoor semi-volatile organic compounds (SVOCs) can have a significant impact on human health. Previous studies involved the detection of limited classes of indoor SVOCs in different regions of China. However, overall indoor pollution profiles and the associated health risks via multiple exposure pathways remain unclear. High-throughput screening of SVOCs would help clarify the overall indoor pollution status and identify high-risk pollutants. We collected indoor air and dust samples from 35 Chinese homes and investigated the occurrence of a wide range of SVOCs. Ninety-seven SVOCs including phthalate esters (PAEs), polycyclic aromatic hydrocarbons (PAHs), organophosphate esters, alcohols, fatty acids, phenols, etc., were detected in the air (total concentrations: 0.13-48 μg/m 3 ; median: 3.4 μg/m 3 ) and dust (total concentrations: 120-1500 μg/g; median: 490 μg/g) samples. PAEs were the most abundant, accounting for 55.3 ± 28.6% and 43.4 ± 16.9% of the total SVOC concentrations in the air and dust samples respectively. Human exposure and health risks of 34 SVOCs with detection frequencies >10% were assessed based on inhalation, ingestion and dermal absorption of SVOCs from air and dust by infants and adults. In the case of indoor SVOCs with log K oa < 9, inhalation and dermal contact with air was >90% for adults and >69% for infants. The following five SVOCs in air samples posed significant non-carcinogenic risks and are listed based on their decreasing risk level: dibutyl phthalate > phenanthrene > stearic acid > methyl palmitate > lauryl alcohol. Four PAHs with 2-4 rings posed potential carcinogenic risks, with phenanthrene exceeding the acceptable risk level of 10 -4 . The high risks posed by SVOCs were due to inhalation exposure. Therefore, keeping the air concentrations of SVOCs, especially that of PAEs and PAHs under check would greatly benefit human health in indoor environments., (Copyright © 2022 Elsevier Ltd. All rights reserved.)

Using an improved multimedia fate model, this study simulated the spatial distributions, partitioning behaviors, and mass exchanges of PAH 16 (16 species with priority by the USEPA) in multiple environmental compartments in the coastal regions of the Bohai and Yellow Seas, Northern China. The model predictions generally matched well with the measured results, as the deviations of most points were within one order of magnitude in the air, freshwater, and 3 soil compartments. The estimated concentrations of ΣPAH 16 in the northern part were higher than those in the southern part, which was consistent with the emissions of each part. Approximately 97.6% of the ΣPAH 16 mass was distributed in soils; therefore, soils served as the dominant sink of PAH 16 . The estimated net flux of ΣPAH 16 from air to soil ranged from 0.4 to 10.7 mg/m 2 /year (an average of 3.2 mg/m 2 /year), and the estimated flux of deposition from air to soil fell in the range of 0.4-10.8 mg/m 2 /year (an average of 3.2 mg/m 2 /year), which served as the dominant process at the air-soil interface. The estimated net flux of ΣPAH 16 from air to freshwater ranged from -15.3 to 9.4 mg/m 2 /year (an average of -0.3 mg/m 2 /year), and the reversed volatilization flux from freshwater to air ranged from 0.01 to 21.1 mg/m 2 /year (an average of 3.7 mg/m 2/ year). This situation indicated notable spatial variations and volatilization as the main process affecting the direction of net flux at the air-freshwater interface. Deterministic risk assessment and probabilistic risk assessment were conducted. The overall health risks of the studied regions were acceptable, while the excess lifetime cancer risk (ELCR) by air inhalation was greater than that by soil ingestion. CAPSULE: Multimedia fate model-predicted distributions and compositions of PAH 16 in different compartments, compartmental exchange fluxes and directions, and deterministic and probabilistic ELCR via different exposure pathways were assessed., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2022 Elsevier B.V. All rights reserved.)

A portable emission sampling system was used to perform on-site measurements of the emission factors (EFs; quantities of pollutants emitted per unit of energy consumed) of 29 polycyclic aromatic hydrocarbons (PAHs) for five types of marine vessels using light diesel in Hainan Province, China. Both gaseous- and particulate-phase PAHs from vessel emissions were sampled and measured using gas chromatography coupled with mass spectrometry (GC-MS), and the PAH EFs were calculated based on the carbon mass balance method. The average EFs of gaseous- and particulate-phase PAHs were 6.2 ± 7.8 and 17 ± 26 mg/kg, with naphthalene (NAP) and phenanthrene (PHE) dominating the gaseous- and particulate-phase PAH emissions, respectively. Among the five types of vessels, the EFs for small fishing boats were significantly higher than those for other types of vessels, and the lowest EFs were found for tug boats. Composition profiles and typical isomer ratios of PAHs were calculated for five types of vessels. Particulate-phase PAHs accounted for 63 ± 16% of the total emissions of 29 PAH species, and the particulate/gaseous-phase partitioning of PAHs was dominated by organic carbon (OC) absorption rather than black carbon (BC) adsorption. Emission factors of PAHs under different activity conditions were measured and calculated, and relatively higher EFs were found in the maneuvering mode for medium fishing boats and in the operating mode for engineering vessels. No significant differences were found among the PAH composition profiles under different activity conditions., (Copyright © 2021 Elsevier Ltd. All rights reserved.)

Industry relocation under globalization has altered the origins and strength of emission sources of many air pollutants. We develop global emission inventories of polycyclic aromatic hydrocarbons (PAHs) embodied in the production and consumption of goods and services. We implement these inventories within a global atmospheric transport model and simulate spatial-temporal changes in atmospheric concentrations of benzo[α]pyrene (BaP), the most toxic congener in unsubstituted PAHs, and depositions across the Arctic subject to global trade and industry relocation. We show that interregional trade and industry relocation dramatically reduce the atmospheric levels and deposition of BaP in the Arctic. The most significant BaP decline occurs in the European and North American Arctic regions due to attenuated sources in the two well-developed continents proximate to the polar region induced by the relocation of high-PAH pollution industries to many developing countries far from the Arctic. Although BaP emissions embodied in industry relocations in China, India, and South and Southeast Asia resulted in increased BaP contamination in the Asian Arctic, such increases in pollution are minor compared to significant BaP reductions occurring in the European and North American Arctic regions. We find that "North-to-South" industry transfer could reduce trade-related BaP contamination by 60% in the Arctic.

China has been famous for its porcelains for millennia, and the combustion processes of porcelain production emit substantial amounts of air pollutants, which have not been well understood. This study provided firsthand data of air pollutant emissions from biomass porcelain kilns. The emission factor of PM 2.5 was 0.95 ± 1.23 g/kg during the entire combustion cycle, lower than that of biomass burning in residential stoves and coal burning in brick kilns, attributed to the removal effects of the long-distance transport in dragon kilns. The temporal trend of particle pollutants, including particulate matters (PMs) and particulate polycyclic aromatic hydrocarbons (PAHs) (low at ignition phase and high at the end) again indicated the removal effects of the special structure, while gaseous pollutants, such as gaseous PAHs, exhibited the opposite result. The GWC 100 was estimated as 1.4 × 10 6 and 0.5 × 10 6  kg CO 2 e/yr for the scenarios in which 50% and 100% of the wood was renewable, respectively. The GWC 100 of dragon kilns is nearly equal to that of 745 households using wood-fueled stoves. These results indicate the necessity of pollution controls for biomass porcelain kilns to estimate the emission inventory and climate change., (Copyright © 2021 Elsevier Ltd. All rights reserved.)

Monte Carlo simulation (MCS) is a computational technique widely used in exposure and risk assessment. However, the result of traditional health risk assessment based on the MCS method has always been questioned due to the uncertainty introduced in parameter estimation and the difficulty in result validation. Herein, data from a large-scale investigation of individual polycyclic aromatic hydrocarbon (PAH) exposure was used to explore the key factors for improving the MCS method. Research participants were selected using a statistical sampling method in a typical PAH polluted city. Atmospheric PAH concentrations from 25 sampling sites in the area were detected by GC-MS and exposure parameters of participants were collected by field measurement. The incremental lifetime cancer risk (ILCR) of participants was calculated based on the measured data and considered to be the actual carcinogenic risk of the population. Predicted risks were evaluated by traditional assessment method based on MCS and three improved models including concentration-adjusted, age-stratified, and correlated-parameter-adjusted Monte Carlo methods. The goodness of fit of the models was evaluated quantitatively by comparing with the actual risk. The results showed that the average risk derived by traditional and age-stratified Monte Carlo simulation was 2.6 times higher, and the standard deviation was 3.7 times higher than the actual values. In contrast, the predicted risks of concentration- and correlated-parameter-adjusted models were in good agreement with the actual ILCR. The results of the comparison suggested that accurate simulation of exposure concentration and adjustment of correlated parameters could greatly improve the MCS. The research also reveals that the social factors related to exposure and potential relationship between variables are important issues affecting risk assessment, which require full consideration in assessment and further study in future research.

Gaseous and particulate nitrated polycyclic aromatic hydrocarbons (NPAHs, 12 species) and oxygenated polycyclic aromatic hydrocarbons (OPAHs, 4 species) in seven coastal cities of the Bohai and Yellow Seas were determined throughout the year. The annual arithmetical mean concentrations of ΣNPAH 12 and ΣOPAH 4 were 737 ± 475 pg/m 3 and 35.3 ± 26.8 ng/m 3 . NPAHs and OPAHs existed mainly in the gaseous phase, accounted for 88.5% and 95.2% of the total concentrations. Air concentrations of ΣNPAH 12 and ΣOPAH 4 in the coastal cities of the Yellow Sea were significantly lower (p < 0.05) than those of the Bohai Sea. Air concentrations of ΣNPAH 12 and ΣOPAH 4 were significantly higher (p < 0.01) in winter than in summer. Strong secondary formation of atmospheric NPAHs and OPAHs occurred in all of the studied cities. The sequence of annual contribution of the emission sources of airborne NPAHs determined by positive matrix factorization was traffic exhaust > combustion of solid fuels (coal and biomass) > secondary formation, while for OPAHs, it was combustion of solid fuels > secondary formation > traffic exhaust. The combustion of solid fuels served as the main source of NPAHs and OPAHs in winter, while secondary formation was the predominant source in summer. Interregional transport may exert an important effect on the local atmospheric NPAHs and OPAHs by potential source contribution function analysis. The estimated incremental lifetime cancer risk (ILCR) due to inhalation exposure to specific NPAHs ranged from 2.9 × 10 -12 to 6.2 × 10 -6 (median at 4.8 × 10 -9 ) was mainly attributed to exposure before the age of 16., (Copyright © 2021 Elsevier Ltd. All rights reserved.)

Polycyclic aromatic hydrocarbons (PAHs) in soil can be recalcitrant to solvent extraction after aging. We showed in this study that mixing a small amount of water in the extracting solvent during microwave-assisted extraction (MAE) can release recalcitrant PAHs, resulting in significant improvement in the analyzed concentrations. The improvement factor (F) for the total of 16 priority PAHs (∑PAH16) listed by the United States Environmental Protection Agency was 1.44-1.55 for field soils. By comparing the F values for different soil organic components, we demonstrated that the recalcitrant PAHs were primarily associated with biochar, humic acid (HA), and humin (HM), with the F values for ∑PAH16 of 1.94, 6.62, and 4.59, respectively. The results showed that the recalcitrant PAHs comprised a sequestered fraction and a desorption-limited fraction. NMR spectra showed that water worked alone at elevated temperature to promote hydrolysis of biochar and destroy the macromolecular structure, thus causing the release of the otherwise sequestered PAHs during MAE. The substantial reduction in F values for HA and HM after demineralization indicated sequestration of PAHs in organic-mineral complexes, which can be destroyed by hot water treatment. The release of the sequestered fraction was nonselective and independent of compound hydrophobicity. In comparison, the release of the desorption-limited fraction was positively affected by the hydrophobicity of PAHs and was facilitated by the presence of water in the extracting solvent. The results of this study provide important insights into the sequestration and release of recalcitrant PAHs in soil., (Copyright © 2021 Elsevier Ltd. All rights reserved.)

Knowledge of the origins of polycyclic aromatic hydrocarbon (PAH) in vegetables is essential to reduce human health risks induced by dietary exposure. The current study developed a vegetation-advanced multimedia model, SESAMe-Veg, to identify the major uptake pathway of 15 priority PAHs in vegetables and assess the PAHs in edible parts of cabbages and carrots in Jinzhong City, Shanxi Province, China. The model was well evaluated against site- and plant-specific measurements. Edible parts exhibited lower PAH concentrations than the other parts for both vegetables. The estimated concentrations of ΣPAH15 were 79 ng/g in cabbage shoots and 83 ng/g in carrot roots. Higher concentrations were estimated in shoots of the leafy vegetable than in roots of the root vegetable for most PAHs. Although air-shoot is the major transport pathway, 98% was deposition of particles, which was attached outside and could be removed relatively easily by washing. Soils might be the origin of PAHs inside vegetables, especially for lighter PAHs. PYR was more likely to be stored in roots than other congeners. The translocation of PAHs inside vegetables was negligible. Adulthood dietary exposure to local vegetables probably caused a high health risk; however, contributions from consuming cabbages and especially carrots were low. Females generally exhibited slightly higher risks than males of exposure to PAHs in local vegetables. Considering the dominant role of particle deposition, carefully vegetable washing before ingestion could reduce this risk. This study has provided a functional tool to evaluate vegetable contamination by PAHs. CAPSULE: A vegetation-advanced multimedia model of PAHs in different parts of vegetables and other environmental media was developed to evaluate the potential health risk to local populations of different sexes and ages via vegetable ingestion., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2021 Elsevier B.V. All rights reserved.)

Residential solid fuel combustion (RSFC) is a key cause of air pollution in China. In these serial studies, field measurements of RSFC from 166 rural households in eastern China were conducted to update the database of emission factors (EFs) and chemical profiles of gaseous and particulate organic pollutants, and the present study focuses on the intermediate volatile organic compounds (IVOCs), which are precursors of secondary organic aerosol (SOA). The results show that the averaged EFs of IVOCs (EF IVOC ) for crop straw, fuelwood, and coal are 550.7 ± 397.9, 416.1 ± 249.5, and 361.9 ± 308.0 mg/kg, respectively, which are among the EF IVOC of gasoline vehicle, diesel vehicle, non-road machinery, and heavy fuel oil vessel, and are significantly affected by fuel, stove, and combustion efficiency. The percentages of normal alkanes ( n -alkanes), branched alkanes ( b -alkanes), polycyclic aromatic hydrocarbons (PAHs), and unresolved complex mixture from RSFC are 3.5 ± 1.6, 8.0 ± 3.7, 17.6 ± 6.7, and 70.9 ± 8.1%, respectively, and the compositions are featured by lower b-alkanes and higher PAHs than those of vehicle sources. The proportions of some individual n-alkanes and PAHs (such as n -C 12 - n -C 15 , naphthalene, and its alkyl substituents) can be used as indicators to differentiate RSFC from vehicle sources, while methoxyphenols can be used to distinguish biomass burning from coal combustion. Based on China's energy statistics, the total IVOC emissions from RSFC in 2014 were 175.9 Gg. These data will help to update the IVOC emission inventory and improve the estimates of SOA production in China.

Indoor biomass burning produces large amounts of small particles and hazardous contaminants leading to severe air pollution and potentially high health risks associated with inhalation exposure. Personal samplers provide more accurate estimates of inhalation exposure. In this study, inhalation exposure to size-segregated particles and particulate polycyclic aromatic hydrocarbons (PAHs) for the biomass user was studied by deploying personal samplers. The study found that daily PM 2.5 inhalation exposure level was as high as 121 ± 96 μg/m 3 , and over 84% was finer PM 1.0 . For PAHs, the exposure level was 113 ± 188 ng/m 3 , with over 77% in PM 1.0 . High molecular weight PAHs with larger toxic potentials enriched in smaller particles resulting in much high risks associated with PAHs inhalation exposure. Indoor exposure contributed to ~80% of the total inhalation exposure as a result of high indoor air pollution and longer residence spent indoor. The highest exposure risk was found for the male smoker who conducted cooking activities at home., (Copyright © 2021 The Authors. Published by Elsevier Inc. All rights reserved.)

Indoor biomass burning is a major contributor to the emission of PAHs (polycyclic aromatic hydrocarbons) in China. To date, estimates of PAH emissions from the burning of biomass have involved considerable uncertainty, mostly from the lack of real-world measurements of emission factors. In this study, we conducted a comprehensive evaluation on PAH emissions from biomass burning in real-world cooking stoves in three Chinese provinces. PAH emission factors, in both particle- and gas-phase, from 11 fuel-stove combinations were measured and the provincial emissions were estimated based on the measured emission factors and fuel consumption. The measured PAH 28 emission factors (including 16 US EPA priority PAHs and 12 non-priority PAHs) ranged from 42 mg/kg to 370 mg/kg, with an order of magnitude difference, which was mostly affected by fuel type. The emission factors measured in this study were generally higher than those reported in laboratory studies and were comparable with field studies. The gas-particle distribution indicated that the absorption of PAHs by organic carbon in particulate matter (PM) was the dominant sorption mechanism in gas-particle distribution. The composition profile was different from previous studies, especially for non-priority PAHs, which are highly toxic and should be given more attention. Following the disparities in composition profiles, our study suggests that source apportionment based on single- or multi-diagnostic ratios may lead to large bias and uncertainties. It appears that the toxicity potential of PAHs in northern China emitted from combustion of crop residues is greater than that in southern China where PAHs are mainly emitted from wood combustion., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2020 Elsevier Ltd. All rights reserved.)

Polycyclic aromatic hydrocarbons (PAHs) are formed by the incomplete combustion of fossil fuels and forest or biomass burning. PAHs undergo long-range atmospheric transport, as evidenced by in situ observations across the Arctic. However, monitored atmospheric concentrations of PAHs indicate that ambient PAH levels in the Arctic do not follow the declining trend of worldwide anthropogenic PAH emissions since the 2000s, suggesting missing sources of PAHs in the Arctic or other places across the Northern Hemisphere. To trace origins and causes for the increasing trend of PAHs in the Arctic, the present study reconstructed PAH emissions from forest fires in the northern boreal forest derived by combining forest carbon stocks and MODIS burned area. We examined the statistical relationships of forest biomass, MODIS burned area, emission factors, and combustion efficiency with different PAH congeners. These relationships were then employed to construct PAH emission inventories from forest biomass burning. We show that for some PAH congeners, for example, benzo[a]pyrene (BaP)-the forest-fire-induced air emissions are almost one order of magnitude higher than previous emission inventories in the Arctic. A global-scale atmospheric chemistry model, GEOS-Chem, was used to simulate air concentrations of BaP, a representative PAH congener primarily emitted from biomass burning, and to quantify the response of BaP to wildfires in the northern boreal forest. The results showed that BaP emissions from wildfires across the northern boreal forest region played a significant role in the contamination and interannual fluctuations of BaP in Arctic air. A source-tagging technique was applied in tracking the origins of BaP pollution from different northern boreal forest regions. We also show that the response of BaP pollution at different Arctic monitoring sites depends on the intensity of human activities., Competing Interests: Declaration of competing interest The authors declare no competing financial interest., (Copyright © 2020 Elsevier Ltd. All rights reserved.)

Gaseous and particulate polycyclic aromatic hydrocarbons (PAHs) and size-segregated particulate matter (PM) in indoor air and outdoor air, along with personal exposure, were monitored in rural households of Northern China. The daily average concentrations of 28 species were 1310 ± 811, 738 ± 321, 465 ± 247, and 655 ± 250 ng/m 3 in kitchen air, bedroom air, and outdoor air, and for personal exposure, respectively. PAHs tended to occur in the particulate phase with increasing molecular weight. Absorption by particulate organic carbon was dominant in the gas-particle partitioning process. The daily averaged concentrations of PM 2.5 and PM 1.0 were 104 ± 39.5 and 88.4 ± 39.3 μg/m 3 in kitchen air, 79.0 ± 63.2 and 65.7 ± 57.5 μg/m 3 in bedroom air, 52.9 ± 16.5 and 41.5 ± 12.5 μg/m 3 in outdoor air, and 71.7 ± 30.8 and 61.5 ± 28.4 μg/m 3 for personal exposure, respectively. The non-priority components contributed 5.5 ± 2.8% to the total PAHs, while their fraction of carcinogenic risk reached 85.6 ± 6.9%. The mean cancer risk posed to rural residents via inhalation exposure to PAHs exceeded the current acceptable threshold of 1.0 × 10 -6 and the national average estimated in China. The personal exposure levels of PAHs and PM in households using clean energy were lower than those in households using traditional biomass by 30.0%, 29.4%, and 38.5% for PAH 28 , PM 2.5 , and PM 1.0 , respectively. However, the cancer risk of personal inhalation exposure to PAH 28 from using liquid petroleum gas (LPG) was higher than that from using firewood, implying the adoption of LPG may not effectively reduce the cancer risk despite the decreasing exposure levels of PAH 28 and PM with respect to the use of firewood. Cooking individuals suffered higher exposure levels of PAH 28 and PM 1.0 compared with non-cooking individuals, and the cancer risk of personal inhalation exposure to PAH 28 for cooking individuals was 1.7 times that for non-cooking individuals. Cooking was a critical factor that affected the personal exposure levels of the local male and female residents., (Copyright © 2019 Elsevier Ltd. All rights reserved.)

Given the lack of understanding of the complex physiochemical and environmental processes of persistent organic pollutants (POPs) in the Arctic and around the globe, atmospheric models often yield large errors in the predicted atmospheric concentrations of POPs. Here, we developed a recurrent neural network (RNN) method based on nonparametric deep learning algorithms. The RNN model was implemented to predict monthly air concentrations of polycyclic aromatic hydrocarbons (PAHs) at the high Arctic monitoring station Alert. To train the RNN system, we used MODIS satellite remotely sensed forest fire data, air emissions, meteorological data, sea ice cover area, and sampled PAH concentration data from 1996 to 2012. The system was applied to forecast monthly PAH concentrations from 2012 to 2014 at the Alert station. The results were compared with monitored PAHs and an atmospheric transport model (CanMETOP) for POPs. We show that the RNN significantly improved PHE and BaP predictions from 2012 to 2014 by 62.5 and 91.1%, respectively, compared to CanMETOP predictions. The sensitivity analysis using the Shapley value reveals that air emissions determined the magnitude of PAH levels in the high Arctic, whereas forest fires played a significant role in the changes in PAH concentrations in the high Arctic, followed by air temperature and meridional wind fields.

Parent polycyclic aromatic hydrocarbons (PPAHs) in the ambient air of the coastal cities near the Bohai and Yellow Seas were measured over a full year. The range and geometric average of total PPAH 29 (29 species) were 5.16-1.22 × 10 3 and 118 ng/m 3 , respectively, with 77 ± 14% in a gaseous phase. The 16 priority components accounted for 90 ± 4% of the total mass concentration. The incremental life cancer risk (ILCR) via inhalation exposure to the PPAHs (3.17 × 10 -4 ) was underestimated by 80%, as only the priority PPAHs were considered. The air concentrations of PPAHs in the Bohai Sea area were generally higher (p < 0.01) than those in the Yellow Sea area. A significant increase (p < 0.01) in the levels of PPAHs and large fractions of high molecular weight (HMW) components were observed in winter. Absorption by particulate organic carbon dominated in gas-particle partitioning of the PPAHs, and the seasonal variations in gas-particle partitioning of the low and moderate molecular weight compounds were more noticeable relative to the HMW species. In summer, significantly higher concentrations of PPAHs were found in the daytime than during nighttime, while the opposite case occurred in winter (p < 0.05). The positive matrix factorization (PMF) results indicated greater contributions of coal and biomass combustion to the PPAH emissions in the coastal cities of the Bohai Sea area compared with the Yellow Sea area. The burning of coal and biomass served as the main source of PPAHs in winter, while traffic exhaust was the dominant source in other seasons. The potential source contribution function (PSCF) revealed the important impacts of the external inputs on the local PPAHs via air mass transport. The contributions of the resolved emission sources to the ILCR were clearly different from those of the mass concentrations, indicating the necessity for source-oriented risk assessments., (Copyright © 2019 Elsevier Ltd. All rights reserved.)

Emission factors (EFs) of polycyclic aromatic hydrocarbon (PAH) derivatives (12 nitro-PAHs and 4 oxy-PAHs) during the pyrolysis of two types of electronic waste (E-waste) were measured. Compositional profile, particle size distribution, gas-particle partitioning, correlations with precursor species and influences of pyrolytic temperature were investigated. The derivative products were dominated by oxy-PAHs. The averaged EFs of oxy-PAHs were 3.37 ± 4.10 μg/g and 32.6 ± 18.1 μg/g for PWBs and plastic casings, respectively, and those of nitro-PAHs were 85.7 ± 92.4 ng/g and 83.3 ± 69.7 ng/g, respectively. Most EFs of derivative species significantly correlated with their corresponding parent PAHs (p < 0.05), except a few cases, indicating formation of derivatives via related reactions of parent species. Most nitro-PAHs occurred in fine particles with the size < 2.1 μm, and oxy-PAHs were prevailing in fine particles with the size between 0.4 μm and 2.1 μm. Proportions of oxy-PAHs in particulate phase, especially those with higher molecular weight, were noticeably greater than those of the corresponding parent species. Below 480 °C, there was no evident difference in the EFs of PAH derivatives, while the EFs noticeably increased from 520 °C. With the increasing temperature, the majority of oxy-PAHs still occurred on finer particles, while the contribution of coarser particles tended to increase., (Copyright © 2019 Elsevier Ltd. All rights reserved.)

Emissions of polycyclic aromatic hydrocarbons (PAHs) in China remain at a high level compared to those in developed countries. The Yangtze River Delta (YRD) is an economic and industrial center in China with an extremely large population. The potentially high emissions and excess cancer risk from human exposure in this region cannot be neglected. This study applied a multimedia model to estimate the concentrations of 16 US EPA priority PAHs in the environment in the YRD with a well-developed PAH-emission inventory for 2014. The model predicted that the average concentrations of ΣPAHs were 274 ng/m 3 in the air, 255 ng/g in the soil, 15 ng/g in vegetation, 147 ng/L in freshwater and 144 ng/g in sediment, as well as 99 ng/L and 80 ng/g in seawater and sediment, respectively. Soil is the PAH sink in this region, and the net flux of the total PAHs is always from air to soil for each isomer. A deterministic assessment observed that the ELCR (excess lifetime cancer risk) ranged from 2.5 × 10 -6 to 3.0 × 10 -5 for exposure by air inhalation and from 3.5 × 10 -7 to 7.9 × 10 -6 for exposure by soil ingestion. The probabilistic results did not find any probability of ELCR >10 -4 by exposure via soil ingestion in the YRD. The probabilistic ELCR induced by inhalation exposure varied from 8.1 × 10 -7 to 3.1 × 10 -4 in the YRD. This study provided a comprehensive overview of PAHs occurrence in natural environments and of the relevant human health risks. The information presented in this study could help authorities to enact a strategy regarding emission reduction and pollution control relevant to PAHs., Capsule: Multimedia modeling predicted distributions and compositions of PAHs in different environmental compartments, and deterministic and probabilistic ELCRs induced by air inhalation and soil ingestion were also provided., (Copyright © 2018 Elsevier B.V. All rights reserved.)

Despite the ubiquity and carcinogenicity of polycyclic aromatic hydrocarbons (PAHs), their dermal absorption for the general population has not been adequately addressed. Aiming to verify the importance of dermal absorption of PAHs, barbecue (BBQ) in Guangzhou, China was chosen as a case study. Urine samples were collected and analyzed for nine hydroxyl (OH)-PAHs. Air, food, and cotton clothing samples were analyzed for 16 PAHs. Dietary exposure was the dominant exposure route with the greatest amounts of OH-PAH excretion and PAH intake. Dermal intake of low molecular-weight PAHs was greater than inhalation intake from the occurrence of atmospheric PAHs. In addition, the net excreted amounts of OH-naphthalene, OH-fluorene, OH-phenanthrene, and OH-pyrene via dermal absorption were 367, 63, 98, and 28 ng, respectively, upon 2.5-h exposure, comparable to those via combined dermal and inhalation exposure, which were 453, 98, 126, and 38 ng. The ratios of excretion to intake via dermal absorption were 0.11, 0.036, and 0.043 for fluorene, phenanthrene, and pyrene, respectively, lower than the ratios from dietary exposure (0.38, 0.14, and 0.060) but higher than the ratios from inhalation (0.097, 0.016, and 0.025). In the case of BBQ fumes, dermal absorption was a more important pathway for intake of low molecular-weight PAHs than inhalation.

A series of field samples including ambient air (gaseous and particulate phases), dust fall, surface soil, rhizosphere soil and cabbage tissues (leaf, root and core), were collected in vegetable bases near a large coking manufacturer in Shanxi Province, Northern China, during a harvest season. A factor analysis was employed to apportion the emission sources of polycyclic aromatic hydrocarbons (PAHs), and the statistical results indicated coal combustion was the dominant emission source that accounted for different environmental media and cabbage tissues, while road traffic, biomass burning and the coking industry contributed to a lesser extent. A structural equation model was first developed to quantitatively explore the transport pathways of PAHs from surrounding media to cabbage tissues. The modeling results showed that PAHs in ambient air were positively associated with those in dust fall, and a close relationship was also true for PAHs in dust fall and in surface soil due to air-soil exchange process. Furthermore, PAHs in surface soil were correlated with those in rhizosphere soil and in the cabbage leaf with the path coefficients of 0.83 and 0.39, respectively. PAHs in the cabbage leaf may dominantly contribute to the accumulation of PAHs in the edible part of cabbages., (Copyright © 2018 Elsevier Ltd. All rights reserved.)

Aging soot in soil under neutral aqueous condition for 30days significantly (p<0.05) reduced the apparent gastrointestinal bioaccessibility (B app ) of polycyclic aromatic hydrocarbons (PAHs) and PAH derivatives (d-PAHs) natively present in a composite fuel soot sample. B app was determined under fasting conditions by a previously developed in vitro digestive model that includes silicone sheet as a third phase absorptive sink in the small intestinal stage. Redistribution of contaminants from soot to soil, determined in independent experiments, was too small to affect B app . Prior uptake by soot of a commercial humic acid representing dissolved soil organic matter had no impact on B app . We identified two causes for the reduction in B app by soil and found they were approximately additive. One is an aging time-independent "matrix effect" attributable to competitive sorption by the soil of labile contaminant that is desorbed from the soot during the digestion test. The other is the dissolution of soluble substances from the soot during the aging process that increases soot surface area and nanoporosity. The increased surface area and nanoporosity drive contaminants from labile to nonlabile states in the soot and decrease the desorption into the digestive fluid, the former contributing most to the reduction in B app . The present study shows that mixing of raw soot with soil has important effects, both aging and non-aging, on the bioaccessibility of soot-borne contaminants., (Copyright © 2017 Elsevier B.V. All rights reserved.)

The quality of agricultural soil is vital to human health, however soil contamination is a severe problem in China. Polycyclic aromatic hydrocarbons (PAHs) have been found to be among the major soil contaminants in China. PAH derivatives could be more toxic but their measurements in soils are extremely limited. This study reports levels, spatial distributions and compositions of 11 nitrated (nPAHs) and 4 oxygenated PAHs (oPAHs) in agricultural soils covering 26 provinces in eastern China to fill the data gap. The excess lifetime cancer risk (ELCR) from the exposure to them in addition to 21 parent PAHs (pPAHs) via soil ingestion has been estimated. The mean concentration of ∑nPAHs and ∑oPAHs in agricultural soils is 50±45μg/kg and 9±8μg/kg respectively. Both ∑nPAHs and ∑oPAHs follow a similar spatial distribution pattern with elevated concentrations found in Liaoning, Shanxi, Henan and Guizhou. However if taking account of pPAHs, the high ELCR by soil ingestion is estimated for Shanxi, Zhejiang, Liaoning, Jiangsu and Hubei. The maximum ELCR is estimated at ca.10 -5 by both deterministic and probabilistic studies with moderate toxic equivalent factors (TEFs). If maximum TEFs available are applied, there is a 0.2% probability that the ELCR will exceed 10 -4 in the areas covered. There is a great chance to underestimate the ELCR via soil ingestion for some regions if only the 16 priority PAHs in agricultural soils are considered. The early life exposure and burden are considered extremely important to ELCR. Emission sources are qualitatively predicted and for areas with higher ELCR such as Shanxi and Liaoning, new loadings of PAHs and derivatives are identified. This is the first large scale study on nPAHs and oPAHs contamination levels in agricultural soils in China. The risk assessment based on this underpins the policy making and is valuable for both scientists and policy makers., (Copyright © 2017 Elsevier Ltd. All rights reserved.)

Alkylated PAHs (APAHs) have been shown to be more toxic and persistent than their non-alkylated parent compounds. However, little is known about the extent of soil contamination by these pollutants. To help understand agricultural soil pollution by these compounds at a regional scale, a total of 18 methylated PAHs (MPAHs, a major class of APAHs) in 243 soil samples were analyzed. These soil samples were collected from 11 sites in the Yangtze River Delta (YRD) region, a representative fast developing area in China. The total concentration of MPAHs (∑18MPAHs) ranged from 5.5 to 696.2 ng/g dry soil, with methylnaphthalenes (M-NAPs) and methylphenanthrenes (M-PHEs) accounting for more than 70% of the compositional profile. Relatively high concentrations of ∑18MPAHs were found in Jiaxing and Huzhou areas of Zhejiang province, as well as on the border between the cities of Wuxi and Suzhou. Different MPAH groups showed dissimilar spatial distribution patterns. The spatial distribution of lower molecular weight MPAHs was related to agricultural straw burning and emissions/depositions from industrial activities, whereas that of higher molecular weight MPAHs was much more a function of the total organic carbon (TOC) content of soil. Although coal, biomass (crop straw and wood), and petroleum combustion were identified to be the major emission sources for most of the sampling sites, the areas with relatively severe pollution with ∑18MPAHs resulted from the localized hotspots of petroleum leakage. Isomeric MPAHs with methyl group substituted at 2- (β) position exhibited significantly higher concentrations than those substituted at 1- (α) position. Results of this work help to understand soil pollution by MPAHs, and are useful for designing effective strategies for pollution control so as to ensure food safety in areas with fast economic growth., (Copyright © 2017 Elsevier Ltd. All rights reserved.)

To elucidate the environmental fate of polycyclic aromatic hydrocarbons (PAHs) once released into soil, sixteen humic acids (HAs) and one humin (HM) fractions were sequentially extracted from a peat soil, and sixteen priority PAHs in these humic substances (HSs) were analyzed. It was found that the total concentration of 16 PAHs (∑16PAHs) increased evidently from HA1 to HA16, and then dramatically reached the highest value in HM. The trend of ∑16PAHs in HAs relates to surface carbon and C-H/C-C contents, the bulk aliphatic carbon content and aliphaticity, as well as the condensation enhancement of carbon domains, which were derived from elemental composition, XPS, 13 C NMR, as well as thermal analyses. HM was identified to be the dominant sink of 16 PAHs retention in soil, due to its aliphatic carbon-rich chemical composition and the highly condensed physical makeup of its carbon domains. This study highlights the joint roles of the physical and chemical properties of HSs in retention of PAHs in soil and the associated mechanisms; the results are of significance for PAH-polluted soil risk assessment and remediation., (Copyright © 2017 Elsevier Ltd. All rights reserved.)

To establish a genetic susceptibility assessment model of lung cancer risk potentially associated with polycyclic aromatic hydrocarbon (PAH) inhalation exposure among non-smokers in China, a total of 143 patients with lung adenocarcinoma and 143 cancer-free individuals were recruited. Sixty-eight genetic polymorphisms in 10 pathways related to PAH metabolism and tumorigenesis were selected and examined. It was observed that 3 genetic polymorphisms, along with 10 additional genetic polymorphisms via gene-gene interactions, significantly influenced lung cancer risk potentially associated with PAH inhalation exposure. Most polymorphisms were associated with PAH metabolism. According to the established genetic susceptibility score (GSS), lung cancer risk increased with a rise in the GSS level, thereby indicating a positive dose-response relationship., (Copyright © 2017 The Editorial Board of Biomedical and Environmental Sciences. Published by China CDC. All rights reserved.)

Plastic pellets and microbes are important constitutes in sediment, but the significance of microbes colonizing on plastic pellets to the environmental fate and transport of organic contaminants has not been adequately recognized and assessed. To address this issue, low-density polyethylene (LDPE), polyoxymethylene (POM) and polypropylene (PP) slices were preloaded with dichlorodiphenyltrichloroethanes (DDTs), polycyclic aromatic hydrocarbons (PAHs) and polychlorinated biphenyls (PCBs) and incubated in abiotic and biotic sediment microcosms. Images from scanning electron microscope, Lysogeny Broth agar plates and confocal laser scanning microscope indicated that all polymer slices incubated in biotic sediments were colonized by microorganisms, particularly the LDPE slices. The occurrence of biofilms induced higher dissipation rates of DDTs and PAHs from the LDPE slice surfaces incubated in the biotic sediments than in the abiotic sediments. Plastic colonization on LDPE slice surfaces enhanced the biotransformation of DDT and some PAHs in both marine and river sediments, but had little impact on PCBs. By comparison, PP and POM with unique properties were shown to exert different impacts on the physical and microbial activities as compared to LDPE. These results clearly demonstrated that the significance of polymer surface affiliated microbes to the environmental fate and behavior of organic contaminants should be recognized.

Samples of ambient air (including gaseous and particulate phases), dust fall, surface soil, rhizosphere soil, core (edible part), outer leaf, and root of cabbage from eight vegetable plots near a large coking manufacturer were collected during the harvest period. Concentrations, compositions, and distributions of parent PAHs in different samples were determined. Our results indicated that most of the parent PAHs in air occurred in the gaseous phase, dominated by low molecular weight (LMW) species with two to three rings. Specific isomeric ratios and principal component analysis were employed to preliminarily identify the local sources of parent PAHs emitted. The main emission sources of parent PAHs could be apportioned as a mixture of coal combustion, coking production, and traffic tailing gas. PAH components with two to four rings were prevailing in dust fall, surface soil, and rhizosphere soil. Concentrations of PAHs in surface soil exhibited a significant positive correlation with topsoil TOC fractions. Compositional profiles in outer leaf and core of cabbage, dominated by LMW species, were similar to those in the local air. Overall, the order of parent PAH concentration in cabbage was outer leaf > root > core. Partial correlation analysis and multivariate linear stepwise regression revealed that PAH concentrations in cabbage core were closely associated with PAHs present both in root and in outer leaf, namely, affected by adsorption, then absorption, and translocation of PAHs from rhizosphere soil and ambient air, respectively.

243 surface soil samples were collected from the Yangtze River Delta (YRD) region, and the concentration distributions and compositional profiles of 27 parent PAHs (PPAHs), nitro- and oxy-derivatives (NPAHs and OPAHs), respectively, and health risk of 16 PPAHs were determined. Atmospheric samples were collected at two sites with high topsoil concentrations of PAHs to assist in identifying the emission sources of PPAHs. The total concentrations of PPAHs, NPAHs and OPAHs fell in the ranges of 21.0-3563.2 ng/g, 0.4-4.6 ng/g and 2.1-834.1 ng/g, respectively. PPAHs in topsoil were dominated by low and medium molecular weight species. The main components of OPAHs were 9FO and ANQ. For NPAHs, only 1N-NAP was frequently detected. Overall, the northern parts of the YRD region were more heavily contaminated by PPAHs and their corresponding derivatives. The soil TOC fraction and GDP per capita were significantly correlated with the spatial distribution of PPAHs. Specific ratios of isomeric species and principal component analysis (PCA) designated combustion of industrial coal and biomass, and traffic exhaust as the main mixed emission sources of PPAHs in surface soils in this region. The detected NPAHs and OPAHs were significantly associated with the corresponding PPAHs. The estimated incremental lifetime cancer risk attributed to 16 PPAHs in surface soil was greater than 10 -6 , indicating a potential risk of contracting cancer by exposure to topsoil from the YRD region. The cumulative probability of cancer risk for both adults and children via three exposure pathways followed the sequence of dermal contact > ingestion > inhalation., (Copyright © 2017 Elsevier Ltd. All rights reserved.)

The total concentrations and component profiles of polycyclic aromatic hydrocarbons (PAHs) in ambient air, surface soil and wheat grain collected from wheat fields near a large steel-smelting manufacturer in Northern China were determined. Based on the specific isomeric ratios of paired species in ambient air, principle component analysis and multivariate linear regression, the main emission source of local PAHs was identified as a mixture of industrial and domestic coal combustion, biomass burning and traffic exhaust. The total organic carbon (TOC) fraction was considerably correlated with the total and individual PAH concentrations in surface soil. The total concentrations of PAHs in wheat grain were relatively low, with dominant low molecular weight constituents, and the compositional profile was more similar to that in ambient air than in topsoil. Combined with more significant results from partial correlation and linear regression models, the contribution from air PAHs to grain PAHs may be greater than that from soil PAHs., (Copyright © 2016. Published by Elsevier B.V.)

Polycyclic aromatic hydrocarbons (PAHs) in agricultural soils, eastern China, were studied through a collection of surface samples at 109 sites. The study covered US EPA priority pollutants but also several non-priority isomers including some dibenzopyrenes which are expected to have higher toxic potentials. The total PAH concentrations varied extensively from 8.8 to 3880 μg/kg, with a geometric mean of 158 μg/kg. There were significant differences in both the concentrations and composition profiles between the south and the north regions. The overall geographical distribution pattern was strongly influenced by both the per capita gross domestic product and soil organic carbon (SOC) content. The former is an indicator of anthropogenic emissions while soil SOC content is associated with the accumulative capacities of the soils. The sequestration mechanism is an important process controlling fates of PAHs in agricultural soil.

Sixteen U.S. EPA priority polycyclic aromatic hydrocarbons (PAHs) and eleven non-priority isomers including some dibenzopyrenes were analyzed to evaluate health risk attributable to inhalation exposure to ambient PAHs and contributions of the non-priority PAHs in a megacity Nanjing, east China. The annual average mass concentration of the total 16 EPA priority PAHs in air was 51.1 ± 29.8 ng/m 3 , comprising up to 93% of the mass concentration of all 27 PAHs, however, the estimated Incremental Lifetime Cancer Risk (ILCR) due to inhalation exposure would be underestimated by 63% on average if only accounting the 16 EPA priority PAHs. The risk would be underestimated by 13% if only particulate PAHs were considered, though gaseous PAHs made up to about 70% of the total mass concentration. During the last fifteen years, ambient Benzo[a]pyrene decreased significantly in the city which was consistent with the declining trend of PAHs emissions. Source contributions to the estimated ILCR were much different from the contributions for the total mass concentration, calling for the introduce of important source-oriented risk assessments. Emissions from gasoline vehicles contributed to 12% of the total mass concentration of 27 PAHs analyzed, but regarding relative contributions to the overall health risk, gasoline vehicle emissions contributed 45% of the calculated ILCR. Dibenzopyrenes were a group of non-priority isomers largely contributing to the calculated ILCR, and vehicle emissions were probably important sources of these high molecular weight isomers. Ambient dibenzo[a,l]pyrene positively correlated with the priority PAH Benzo[g,h,i]perylene. The study indicates that inclusion of non-priority PAHs could be valuable for both PAH source apportionment and health risk assessment., (Copyright © 2017 Elsevier Ltd. All rights reserved.)

Residential solid fuels are widely consumed in rural China, contributing to severe household air pollution for many products of incomplete combustion, such as polycyclic aromatic hydrocarbons (PAHs) and their polar derivatives. In this study, concentrations of nitrated and oxygenated PAH derivatives (nPAHs and oPAHs) for household and personal air were measured and analyzed for influencing factors like smoking and cooking energy type. Concentrations of nPAHs and oPAHs in kitchens were higher than those in living rooms and in outdoor air. Exposure levels measured by personal samplers were lower than levels in indoor air, but higher than outdoor air levels. With increasing molecular weight, individual compounds tended to be more commonly partitioned to particulate matter (PM); moreover, higher molecular weight nPAHs and oPAHs were preferentially found in finer particles, suggesting a potential for increased health risks. Smoking behavior raised the concentrations of nPAHs and oPAHs in personal air significantly. People who cooked food also had higher personal exposures. Cooking and smoking have a significant interaction effect on personal exposure. Concentrations in kitchens and personal exposure to nPAHs and oPAHs for households using wood and peat were significantly higher than for those using electricity and liquid petroleum gas (LPG)., (© 2016 John Wiley & Sons A/S. Published by John Wiley & Sons Ltd.)

Mass transfer of hydrophobic organic contaminants (HOCs) across the air-water interface is an important geochemical process controlling the fate and transport of HOCs at the regional and global scales. However, few studies have characterized concentration or fugacity profiles of HOCs near both sides of the air-water interface, which is the driving force for the inter-compartmental mass transfer of HOCs. Herein, we introduce a novel passive sampling device which is capable of measuring concentration (and therefore fugacity) gradients of HOCs across the air-water interface. Laboratory studies indicated that the escaping fugacity values of polycyclic aromatic hydrocarbons (PAHs) from water to air were negatively correlated to their volatilization half-lives. Results for field deployment were consistent between the passive sampler and an active method, i.e., a combination of grab sampling and liquid-liquid extraction. In general, the fugacity profiles of detected PAHs were indicative of an accumulation mechanism in the surface microlayer of the study regions (Haizhu Lake and Hailing Bay of Guangdong Province, China), while p,p'-DDD tended to volatilize from water to the atmosphere in Hailing Bay. Furthermore, the fugacity profiles of the target analytes increased towards the air-water interface, reflecting the complexity of environmental behavior of the target analytes near the air-water interface. Overall, the passive sampling device provides a novel means to better characterize the air-water diffusive transfer of HOCs, facilitating the understanding of the global cycling of HOCs., (Copyright © 2016 Elsevier Ltd. All rights reserved.)

Ingestion of soot present in soil or other environmental particles is expected to be an important route of exposure to nitro and oxygenated derivatives of polycyclic aromatic hydrocarbons (PAHs). We measured the apparent bioaccessibility (B app ) of native concentrations of 1-nitropyrene (1N-PYR), 9-fluorenone (9FLO), anthracene-9,10-dione (ATQ), benzo[a]anthracene-7,12-dione (BaAQ), and benzanthrone (BZO) in a composite fuel soot sample using a previously-developed in vitro human gastrointestinal model that includes silicone sheet as a third-phase absorptive sink. Along with B app , we determined the 24-h sheet-digestive fluid partition coefficient (K s,24h ), the soot residue-fluid distribution ratio of the labile sorbed fraction after digestion (K r,lab ), and the maximum possible (limiting) bioaccessibility, B lim . The B app of PAH derivatives was positively affected by the presence of the sheet due to mass-action removal of the sorbed compounds. In all cases B app increased with imposition of fed conditions. The enhancement of B app under fed conditions is due to increasingly favorable mass transfer of target compounds from soot to fluid (increasing bile acid concentration, or adding food lipids) or transfer from fluid to sheet (by raising small intestinal pH). Food lipids may also enhance B app by mobilizing contaminants from nonlabile to labile states of the soot. Compared to the parent PAH, the derivatives had larger K r,lab , despite having lower partition coefficients to various hydrophobic reference phases including silicone sheet. The B lim of the derivatives under the default conditions of the model ranged from 65.5% to 34.4%, in the order, 1N-PYR > ATQ > 9FLO > BZO > BaAQ, with no significant correlation with hydrophobic parameters, nor consistent relationship with B lim of the parent PAH. Consistent with earlier experiments on a wider range of PAHs, the results suggest that a major determinant of bioaccessibility is the distribution of chemical between nonlabile and labile states in the original solid., (Copyright © 2016 Elsevier Ltd. All rights reserved.)

Polycyclic aromatic hydrocarbons (PAHs) derivatives like nitrated and oxygenated PAHs are of growing concerns because of considerably higher toxicity and important roles during atmospheric chemical reactions. Residential solid fuel combustion is likely to be one large primary source of these pollutants in developing countries. In this study, inhalation exposure to nitrated and oxygenated PAH derivatives was evaluated among rural residents using carried samplers. The exposure levels of individual nitrated PAHs ranged from 4.04 (9-nitrated phenanthrene) to 89.8 (9-nitrated anthracene) pg/m(3), and of oxy-PAHs were 0.570 (benzo[a]anthracene-7, 12-dione) to 7.99 (Benzanthrone) ng/m(3), generally higher in wood user than that in anthracite user. A majority of derivatives in particle presented in PM2.5 (80% for nitrated naphthalene and over 90% for other targets) and even fine PM1.0. Mass fractions of PAH derivatives in fine and ultra-fine particles were significantly higher than the fractions of corresponding parent PAHs, indicating more adverse health outcomes induced by these derivatives. The inhalation exposure levels for residents adopting wood gasifier burners was significantly lower than the documented results for those burning wood in typical built-in brick stoves, and comparable to those using LPG and electricity, which provided vital information for clean stove development and intervention programs., (Copyright © 2016 Elsevier Ltd. All rights reserved.)

Polycyclic aromatic hydrocarbons (PAHs) are often detected in the environment and are regarded as endocrine disruptors. We here designated mixtures of PAHs in the environment as environmental PAHs (ePAHs) to discuss their effects collectively, which could be different from the sum of the constituent PAHs. We first summarized the biological impact of environmental PAHs (ePAHs) found in the atmosphere, sediments, soils, and water as a result of human activities, accidents, or natural phenomena. ePAHs are characterized by their sources and forms, followed by their biological effects and social impact, and bioassays that are used to investigate their biological effects. The findings of the bioassays have demonstrated that ePAHs have the ability to affect the endocrine systems of humans and animals. The pathways that mediate cell signaling for the endocrine disruptions induced by ePAHs and PAHs have also been summarized in order to obtain a clearer understanding of the mechanisms responsible for these effects without animal tests; they include specific signaling pathways (MAPK and other signaling pathways), regulatory mechanisms (chromatin/epigenetic regulation, cell cycle/DNA damage control, and cytoskeletal/adhesion regulation), and cell functions (apoptosis, autophagy, immune responses/inflammation, neurological responses, and development/differentiation) induced by specific PAHs, such as benz[a]anthracene, benzo[a]pyrene, benz[l]aceanthrylene, cyclopenta[c,d]pyrene, 7,12-dimethylbenz[a]anthracene, fluoranthene, fluorene, 3-methylcholanthrene, perylene, phenanthrene, and pyrene as well as their derivatives. Estrogen signaling is one of the most studied pathways associated with the endocrine-disrupting activities of PAHs, and involves estrogen receptors and aryl hydrocarbon receptors. However, some of the actions of PAHs are contradictory, complex, and unexplainable. Although several possibilities have been suggested, such as direct interactions between PAHs and receptors and the suppression of their activities through other pathways, the mechanisms underlying the activities of PAHs remain unclear. Thus, standardized assay protocols for pathway-based assessments are considered to be important to overcome these issues., (Copyright © 2016 Elsevier Ltd. All rights reserved.)

Polycyclic aromatic hydrocarbons (PAHs) are a group of pollutants of widespread concerns. Gaseous and size-segregated particulate-phase PAHs were collected in indoor and outdoor air in rural households. Personal exposure was measured and compared to the ingestion exposure. The average concentrations of 28 parent PAHs and benzo(a)pyrene (BaP) were 9000 ± 8390 and 131 ± 236 ng/m(3) for kitchen, 2590 ± 2270 and 43 ± 95 ng/m(3) for living room, and 2800 ± 3890 and 1.6 ± 0.7 ng/m(3) for outdoor air, respectively. The mass percent of high molecular weight (HMW) compounds with 5-6 rings contributed 1.3% to total 28 parent PAHs. Relatively higher fractions of HMW PAHs were found in indoor air compared to outdoor air. Majorities of particle-bound PAHs were found in the finest PM0.25 , and the highest levels of fine PM0.25 -bound PAHs were in the kitchen using peat and wood as energy sources. The 24-h personal PAH exposure concentration was 2100 ± 1300 ng/m(3) . Considering energies, exposures to those using wood were the highest. The PAH inhalation exposure comprised up to about 30% in total PAH exposure through food ingestion and inhalation, and the population attributable fraction (PAF) for lung cancer in the region was 0.85%. The risks for inhaled and ingested intakes of PAHs were 1.0 × 10(-5) and 1.1 × 10(-5) , respectively., (© 2015 John Wiley & Sons A/S. Published by John Wiley & Sons Ltd.)

In this study, paired surface soil and mature wheat grain samples were collected in the cornfields near the large Handan Steel Manufacturer; and the total concentrations and compositional profiles of the parent PAHs were measured, then the spatial distribution characteristics and correlation with total organic carbon fractions in soil were determined. Accordingly, a preliminary source identification was performed, and the association between PAHs in surface soil and wheat grain was briefly discussed. The median concentration of total PAHs in surface soils from the cornfields of Handan was 398.9 ng x g(-1) (ranged from 123.4 ng x g(-1) to 1626.4 ng x g(-1), where around 18% and 10% of all the studied soil samples were over the corresponding quality criteria for total PAHs and B [a] P in soils, respectively. The MMW and HMW species were the main components in the compositional profiles of surface soils. Based on the specific isomeric ratios of PAHs species, coal/biomass combustion and transportation fuel (tail gas) were the dominant mixed sources for the local PAHs emission. The fractions of surface soil TOC had significant positive correlations with the total PAHs and also with the individual components with different rings. In addition, the median concentration of total PAHs in wheat grains collected in the cornfields near the Handan Steel Manufacture was 27.0 ng x g(-1) (ranged from 19.0-34.0 ng x g(-1)). The levels in wheat grains were not high, and lower than the related hygienic standards of food proposed by EU and China. The LMW and MMW PAHs with 2 to 4 rings occupied a larger proportion, more than 84% of the total PAHs, which was largely different from the component profiles in surface soils. This situation suggested that the local sources of PAHs in wheat grains may originate not only from surface soil via root absorption and internal transportation, but also from ambient air through dry and wet deposition on the leaf surface (stoma).

We investigated the effects of changing physiological conditions in the digestive tract expected with food ingestion on the apparent bioaccessibility (Bapp) of 11 polycyclic aromatic hydrocarbons (PAHs) in a fuel soot. A previously established in vitro digestive model was applied that included silicone sheet as a third-phase absorptive sink simulating passive transfer of PAHs to intestinal epithelium in the small intestine stage. The Bapp is defined as the fraction found in the digestive fluid plus sheet after digestion. We determined that Bapp was independent of gastric pH and addition of nonlipid milk representing dietary proteins and carbohydrates, whereas it increased with bile acids concentration (2.0-10 g/L), small intestinal pH (5.00-7.35), and addition of soybean oil representing dietary lipid (100% and 200% of the mean daily ingestion by 2-5 year olds in the U.S.). Bapp of PAHs increases with small intestinal pH due to the combined effects of mass transfer promotion from nonlabile to labile sorbed states in the soot, weaker sorption of the labile state, and increasingly favorable partitioning from the digestive fluid to the silicone sink. Under fed conditions, Bapp increases with inclusion of lipids due to the combined effects of mass transfer promotion from nonlabile to labile states, and increasingly favorable partitioning into bile acid micelles. Our results indicate significant variability in soot PAH bioaccessibility within the range of physiological conditions experienced by humans, and suggest that bioaccessibility will increase with coconsumption of food, especially food with high fat content.

The concentrations and composition of sixteen PAHs adsorbed to respirable particulate matter (PM10≤10 μm) and inhalable particulate matter (PM2.5≤2.5 μm) were determined during autumn and winter in rural households of Henan Province, China, which used four types of domestic energy [crop residues, coal, liquid petroleum gas (LPG) and electricity] for cooking and heating. The present results show that there were significantly (p<0.05) seasonal variations of particulate-bound PAHs in the rural households. The daily mean concentrations of particulate-bound PAHs in the kitchens, sitting rooms and outdoors were apparently higher in winter than those in autumn, except those in the kitchens using coal. The present study also shows that there were obvious variations of particulate-bound PAHs among the four types of domestic energy used in the rural households. The households using LPG for cooking can, at least in some circumstances, have higher concentrations of PAHs in the kitchens than using crop residues or electricity. In addition, using coal in the sitting rooms seemed to result in apparently higher concentrations of particulate-bound PAHs than using the other three types of domestic energy during winter. The most severe contamination occurred in the kitchens using LPG in winter, where the daily mean concentrations of PM2.5-bound PAHs were up to 762.5±931.2 ng m(-3), indicating that there was serious health risk of inhalation exposure to PAHs in the rural households of Henan Province. Rural residents' exposure to PM2.5-bound PAHs in kitchens would be roughly reduced by 69.8% and 85.5% via replacing coal or crop residues with electricity in autumn. The pilot research would provide important supplementary information to the indoor air pollution studies in rural area., (Copyright © 2015 Elsevier B.V. All rights reserved.)

Polycyclic aromatic hydrocarbons (PAHs) can cause adverse effects on human health. The relative contributions of their two major intake routes (diet and inhalation) to population PAH exposure are still unclear. We modeled the contributions of diet and inhalation to the overall PAH exposure of the population of Beijing in China, and assessed their human incremental lifetime cancer risks (ILCR) using a Mont Carlo simulation approach. The results showed that diet accounted for about 85% of low-molecular-weight PAH (L-PAH) exposure, while inhalation accounted for approximately 57% of high-molecular-weight PAH (H-PAH) exposure of the Beijing population. Meat and cereals were the main contributors to dietary PAH exposure. Both gaseous- and particulate-phase PAHs contributed to L-PAH exposure through inhalation, whereas exposure to H-PAHs was mostly from the particulate-phase. To reduce the cancer incidence of the Beijing population, more attention should be given to inhaled particulate-phase PAHs with considerable carcinogenic potential., (Copyright © 2015 Elsevier Ltd. All rights reserved.)

There is wide concern about polycyclic aromatic hydrocarbons (PAHs) because of their carcinogenic and mutagenic potential. The coking industry is an important source of PAHs. In this study, 36 arable soil samples, a sensitive medium from the perspective of food safety and health, were collected from one of the largest coke production bases in China. The concentration of total 21 PAHs ranged from 294 to 1665 ng g(-1), with a mean of 822±355 ng g(-1). Approximately 60% of the soil samples were heavily polluted with the level higher than 600 ng g(-1). Particularly high abundances of high molecular weight PAHs were found, and the calculated BaPeq was as high as 54.3 ng g(-1). Soil PAH levels were positively correlated with soil organic matter content. The soil PAHs were from complex mixture sources, and high-temperature pyrogenic sources were most likely responsible for the heavy PAH contamination. Effective control strategies and probable remediation approaches should be proposed to improve soil quality., (Copyright © 2015 Elsevier Ltd. All rights reserved.)

Polycyclic aromatic hydrocarbons (PAHs) associated with soot or black carbon can enter the human digestive tract by unintentional ingestion of soil or other particles. This study investigated the bioaccessibility of 11 PAHs in a composite fuel soot sample using an in vitro digestive model that included silicone sheet as an absorptive sink during the small intestinal digestion stage. The sheet was meant to simulate the passive transfer of PAHs in lumen fluid across the small intestinal epithelium, which was postulated to promote desorption of labile PAHs from the soot by steepening the soot-fluid concentration gradient. We show that the presence of silicone sheet during a 4 h default digestion time significantly increased the apparent bioaccessible fraction (Bapp, %), defined as the sum in the sheet and digestive fluid relative to the total PAH determined. The ability to increase Bapp for most PAHs leveled off above a sheet-to-soot ratio of 2.0 g per 50 mg, indicating that the sheet is an effective absorptive sink and promotes desorption in the mentioned way. Enhancement of Bapp by the sheet correlated positively with the octanol-water partition coefficient (Kow), even though the partition coefficient of PAH between sheet and digestive fluid (which contains bile acid micelles) correlated negatively with Kow. It was hypothesized that PAHs initially in the soot exist in labile and nonlabile states. The fraction of labile PAH still sorbed to the soot residue after digestion, and the maximum possible (limiting) bioaccessibility (Blim) could be estimated by varying the sheet-to-soot ratio. We show conclusively that the increase in bioccessibility due to the presence of the sheet is accounted for by a corresponding decrease in fraction of labile PAH still sorbed to the soot. The Blim ranged from 30.8 to 62.4%, independent of molecular size. The nonlabile fraction of individual PAHs (69.2-37.6% in this case) is therefore large and needs to be taken into account in risk assessment.

Twelve nitro-PAHs (nPAHs) and four oxy-PAHs (oPAHs) were measured in air samples for 12 months at 18 sites in urban settings, rural villages, or rural fields in northern China. The nPAH concentrations were higher in urban areas (1.3 ± 1.3 ng/m(3)), and nPAH/parent PAH ratios were higher (suggesting important contributions from motor vehicles and secondary formation) in urban sites than in rural villages. oPAHs are primarily emitted from solid fuel combustion and motor vehicles, and similar oPAH concentrations were found in urban areas (23 ± 20 ng/m(3)) and rural villages (29 ± 24 ng/m(3)). The high numbers of motor vehicles in Beijing and intensive industrial activity in Taiyuan and Dezhou caused higher nPAH concentrations. No spatial trend in oPAH concentrations was found in the rural villages, because similar oPAH mixtures are emitted from solild fuel combustion. The nPAH and oPAH concentrations were higher in the winter, and correlated with residential energy consumption and precipitation., (Copyright © 2014 Elsevier Ltd. All rights reserved.)