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Ultrafine particles (UFP) are the smallest atmospheric particulate matter linked to air pollution-related diseases. The extent to which UFP's physical and chemical properties contribute to its toxicity remains unclear. It is hypothesized that UFP act as carriers for chemicals that drive biological responses. This study explores robust methods for generating reference UFP to understand these mechanisms and perform toxicological tests. Two types of combustion-related UFP with similar elemental carbon cores and physical properties but different organic loads were generated and characterized. Human alveolar epithelial cells were exposed to these UFP at the air-liquid interface, and several toxicological endpoints were measured. UFP were generated using a miniCAST under fuel-rich conditions and immediately diluted to minimize agglomeration. A catalytic stripper and charcoal denuder removed volatile gases and semi-volatile particles from the surface. By adjusting the temperature of the catalytic stripper, UFP with high and low organic content was produced. These reference particles exhibited fractal structures with high reproducibility and stability over a year, maintaining similar mass and number concentrations (100 μg/m 3 , 2.0·10 5 #/cm 3 ) and a mean particle diameter of about 40 nm. High organic content UFP had significant PAH levels, with benzo[a]pyrene at 0.2 % (m/m). Toxicological evaluations revealed that both UFP types similarly affected cytotoxicity and cell viability, regardless of organic load. Higher xenobiotic metabolism was noted for PAH-rich UFP, while reactive oxidation markers increased when semi-volatiles were stripped off. Both UFP types caused DNA strand breaks, but only the high organic content UFP induced DNA oxidation. This methodology allows modification of UFP's chemical properties while maintaining comparable physical properties, linking these variations to biological responses., 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 © 2024 The Authors. Published by Elsevier B.V. All rights reserved.)

In this study, we propose a novel long short-term memory (LSTM) neural network model that leverages color features (HSV: hue, saturation, value) extracted from street images to estimate air quality with particulate matter (PM) in four typical European environments: urban, suburban, villages, and the harbor. To evaluate its performance, we utilize concentration data for eight parameters of ambient PM (PM 1.0 , PM 2.5 , and PM 10 , particle number concentration, lung-deposited surface area, equivalent mass concentrations of ultraviolet PM, black carbon, and brown carbon) collected from a mobile monitoring platform during the nonheating season in downtown Augsburg, Germany, along with synchronized street view images. Experimental comparisons were conducted between the LSTM model and other deep learning models (recurrent neural network and gated recurrent unit). The results clearly demonstrate a better performance of the LSTM model compared with other statistically based models. The LSTM-HSV model achieved impressive interpretability rates above 80%, for the eight PM metrics mentioned above, indicating the expected performance of the proposed model. Moreover, the successful application of the LSTM-HSV model in other seasons of Augsburg city and various environments (suburbs, villages, and harbor cities) demonstrates its satisfactory generalization capabilities in both temporal and spatial dimensions. The successful application of the LSTM-HSV model underscores its potential as a versatile tool for the estimation of air pollution after presampling of the studied area, with broad implications for urban planning and public health initiatives.

The emissions of marine diesel engines have gained both global and regional attentions because of their impact on human health and climate change. To reduce ship emissions, the International Maritime Organization capped the fuel sulfur content of marine fuels. Consequently, either low-sulfur fuels or additional exhaust gas cleaning devices for the reduction in sulfur dioxide (SO 2 ) emissions became mandatory. Although a wet scrubber reduces the amount of SO 2 significantly, there is still a need to consider the reduction in particle emissions directly. We present data on the particle removal efficiency of a scrubber regarding particle number and mass concentration with different marine fuel types, marine gas oil, and two heavy fuel oils (HFOs). An open-loop sulfur scrubber was installed in the exhaust line of a marine diesel test engine. Fine particulate matter was comprehensively characterized in terms of its physical and chemical properties. The wet scrubber led up to a 40% reduction in particle number, whereas a reduction in particle mass emissions was not generally determined. We observed a shift in the size distribution by the scrubber to larger particle diameters when the engine was operated on conventional HFOs. The reduction in particle number concentrations and shift in particle size were caused by the coagulation of soot particles and formation/growing of sulfur-containing particles. Combining the scrubber with a wet electrostatic precipitator as an additional abatement system showed a reduction in particle number and mass emission factors by >98%. Therefore, the application of a wet scrubber for the after-treatment of marine fuel oil combustion will reduce SO 2 emissions, but it does not substantially affect the number and mass concentration of respirable particulate matters. To reduce particle emission, the scrubber should be combined with additional abatement systems., 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 Ltd. All rights reserved.)

This study aimed to evaluate the levels and phenomenology of equivalent black carbon (eBC) at the city center of Augsburg, Germany (01/2018 to 12/2020). Furthermore, the potential health risk of eBC based on equivalent numbers of passively smoked cigarettes (PSC) was also evaluated, with special emphasis on the impact caused by the COVID19 lockdown restriction measures. As it could be expected, peak concentrations of eBC were commonly recorded in morning (06:00-8:00 LT) and night (19:00-22:00 LT) in all seasons, coinciding with traffic rush hours and atmospheric stagnation. The variability of eBC was highly influenced by diurnal variations in traffic and meteorology (air temperature (T), mixing-layer height (MLH), wind speed (WS)) across days and seasons. Furthermore, a marked "weekend effect" was evidenced, with an average eBC decrease of ∼35% due to lower traffic flow. During the COVID19 lockdown period, an average ∼60% reduction of the traffic flow resulted in ∼30% eBC decrease, as the health risks of eBC exposure was markedly reduced during this period. The implementation of a multilinear regression analysis allowed to explain for 53% of the variability in measured eBC, indicating that the several factors (e.g., traffic and meteorology) may contribute simultaneously to this proportion. Overall, this study will provide valuable input to the policy makers to mitigate eBC pollutant and its adverse effect on environment and human health., 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 Ltd. All rights reserved.)

Background: Exposure to air pollutants is one of the major environmental health risks faced by populations globally. Information about inhaled particle deposition dose is crucial in establishing the dose-response function for assessing health-related effects due to exposure to air pollution., Objective: This study aims to quantify the respiratory tract deposition (RTD) of equivalent black carbon (BC) particles in healthy young adults during a real-world commuting scenario, analyze factors affecting RTD of BC, and provide key parameters for the assessment of RTD., Methods: A novel in situ method was applied to experimentally determine the RTD of BC particles among subjects in the highly polluted megacity of Metro Manila, Philippines. Exposure measurements were made for 40 volunteers during public transport and walking., Results: The observed BC exposure concentration was up to 17-times higher than in developed regions. The deposition dose rate (DDR) of BC was up to 3 times higher during commute inside a public transport compared to walking (11.6 versus 4.4 μg hr -1 , respectively). This is twice higher than reported in similar studies. The average BC mass deposition fraction (DF) was found to be 43 ± 16%, which can in large be described by individual factors and does not depend on gender., Conclusions: Commuting by open-sided public transport, commonly used in developing regions, poses a significant health risk due to acquiring extremely high doses of carcinogenic traffic-related pollutants. There is an urgent need to drastically update air pollution mitigation strategies for reduction of dangerously high emissions of BC in urban setting in developing regions. The presented mobile measurement set-up to determine respiratory tract deposition dose is a practical and cost-effective tool that can be used to investigate respiratory deposition in challenging environments., (© 2022. The Author(s).)

Background: Secondary organic aerosols (SOAs) formed from anthropogenic or biogenic gaseous precursors in the atmosphere substantially contribute to the ambient fine particulate matter [PM ≤ 2.5 μ m in aerodynamic diameter ( PM 2.5 )] burden, which has been associated with adverse human health effects. However, there is only limited evidence on their differential toxicological impact., Objectives: We aimed to discriminate toxicological effects of aerosols generated by atmospheric aging on combustion soot particles (SPs) of gaseous biogenic ( β -pinene ) or anthropogenic (naphthalene) precursors in two different lung cell models exposed at the air-liquid interface (ALI)., Methods: Mono- or cocultures of lung epithelial cells (A549) and endothelial cells (EA.hy926) were exposed at the ALI for 4 h to different aerosol concentrations of a photochemically aged mixture of primary combustion SP and β -pinene ( SOA β PIN -SP ) or naphthalene ( SOA NAP -SP ). The internally mixed soot/SOA particles were comprehensively characterized in terms of their physical and chemical properties. We conducted toxicity tests to determine cytotoxicity, intracellular oxidative stress, primary and secondary genotoxicity, as well as inflammatory and angiogenic effects., Results: We observed considerable toxicity-related outcomes in cells treated with either SOA type. Greater adverse effects were measured for SOA NAP -SP compared with SOA β PIN -SP in both cell models, whereas the nano-sized soot cores alone showed only minor effects. At the functional level, we found that SOA NAP -SP augmented the secretion of malondialdehyde and interleukin-8 and may have induced the activation of endothelial cells in the coculture system. This activation was confirmed by comet assay, suggesting secondary genotoxicity and greater angiogenic potential. Chemical characterization of PM revealed distinct qualitative differences in the composition of the two secondary aerosol types., Discussion: In this study using A549 and EA.hy926 cells exposed at ALI, SOA compounds had greater toxicity than primary SPs. Photochemical aging of naphthalene was associated with the formation of more oxidized, more aromatic SOAs with a higher oxidative potential and toxicity compared with β -pinene . Thus, we conclude that the influence of atmospheric chemistry on the chemical PM composition plays a crucial role for the adverse health outcome of emissions. https://doi.org/10.1289/EHP9413.

This study analyzed long-term observational data of particulate matter (PM 2.5 , PM 10 ) variability, gaseous pollutants (CO, NO 2 , NO X , SO 2 , and O 3 ), and meteorological factors in 412 fixed monitoring stations from January 2008 to December 2018 in Germany. Based on Hurst index analysis, the trend of atmospheric pollutants in Germany was stable during the research period. The relative correlations of gaseous pollutants and meteorological factors on PM 2.5 and PM 10 concentrations were analyzed by Back Propagation Neural Network model, showing that CO and temperature had the greater correlations with PM 2.5 and PM 10 . Following that, PM 2.5 and PM 10 show a strong positive correlation (R 2  = 0.96, p < 0.01), suggesting that the reduction of PM 2.5 is essential for reducing PM pollution and enhancing air quality in Germany. Based on typical PM 10 /CO ratios obtained under ideal weather conditions, it is conducive to roughly estimate the contribution of natural sources. In winter, the earth's crust contributed about 20.1% to PM 10 . Taken together, exploring the prediction methods and analyzing the characteristic variation of pollutants will contribute an essential implication for air quality control in Germany., 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 Ltd. All rights reserved.)

The study investigates the spatial pattern of black carbon (BC) at a high spatial resolution in Augsburg, Germany. Sixty two walks were performed to assess the concentrations of equivalent black carbon (eBC), ultraviolet particulate matter (UVPM), and equivalent brown carbon (eBrC) in different seasons and at different times of the day with a mobile platform (i.e., trolley). Along with BC measurements, images of street microenvironments were recorded. Meteorological parameters, including temperature, relative humidity, and wind speed, were monitored. The BC concentrations showed significant spatial heterogeneity and diurnal variations peaking in the morning and at night. The highest BC concentrations were observed near dense traffic. The correlations between BC and street views (buildings, roads, cars, and vegetation) were weak but highly significant. Moreover, meteorological factors also influenced the BC concentration. A model based on street view images and meteorological data was developed to examine the driving factors of the spatial variability of BC concentrations at a higher spatial resolution as different microenvironments based on traffic density. The best results were obtained for UVPM and eBC (71 and 70% explained variability). eBrC (53%), to which other sources besides road traffic can also make significant contributions, is modeled less well.

Exceeding the maximum levels for environmental pollutants creates public and scientific interest for the environmental and human health impact it may have. In Northern Italy, the Po Valley, and in particular the Veneto region, is still a hotspot for air quality improvement. Several monitoring campaigns were carried out in this area to acquire information about sources of pollutants which are considered critical. For the first time, a deep study of the aerosol organic fraction was performed in the town Sernaglia della Battaglia, nearby Treviso. During three seasons of 2017, PM 1 and PM 2.5 samples were collected simultaneously. Organic molecular markers have been analyzed by in-situ derivatization thermal desorption gas chromatography time-of-flight mass spectrometry (IDTD-GC-TOFMS). Alkanes, polycyclic aromatic hydrocarbons, oxi-polycyclic aromatic hydrocarbons, anhydrous sugars, resins acids, triterpenoids, and acids were considered. The organic chemical composition has been analyzed based on seasonal variation and source contributions. Principal Component Analysis (PCA) and Positive Matrix Factorization (PMF) have been combined to deeply investigate the main sources of particulate organic matter. On the one hand, PCA evaluates the correlations between the organic markers and their seasonal distribution. On the other hand, the source contributions to aerosol composition are estimated by PMF. Four main emission sources were found by PMF: solid fuel combustion (coal, wood), combustion of petroleum distillates (gas and fuel oil) and exhaust gases of vehicles, industrial combustion processes, home heating, and forest fires are evaluated as the most important sources for the air quality and pollution in this municipality of Northern Italy., 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 Inc. All rights reserved.)

Background: Wood combustion emissions have been studied previously either by in vitro or in vivo models using collected particles, yet most studies have neglected gaseous compounds. Furthermore, a more accurate and holistic view of the toxicity of aerosols can be gained with parallel in vitro and in vivo studies using direct exposure methods. Moreover, modern exposure techniques such as air-liquid interface (ALI) exposures enable better assessment of the toxicity of the applied aerosols than, for example, the previous state-of-the-art submerged cell exposure techniques., Methods: We used three different ALI exposure systems in parallel to study the toxicological effects of spruce and pine combustion emissions in human alveolar epithelial (A549) and murine macrophage (RAW264.7) cell lines. A whole-body mouse inhalation system was also used to expose C57BL/6 J mice to aerosol emissions. Moreover, gaseous and particulate fractions were studied separately in one of the cell exposure systems. After exposure, the cells and animals were measured for various parameters of cytotoxicity, inflammation, genotoxicity, transcriptome and proteome., Results: We found that diluted (1:15) exposure pine combustion emissions (PM 1 mass 7.7 ± 6.5 mg m - 3 , 41 mg MJ - 1 ) contained, on average, more PM and polycyclic aromatic hydrocarbons (PAHs) than spruce (PM 1 mass 4.3 ± 5.1 mg m - 3 , 26 mg MJ - 1 ) emissions, which instead showed a higher concentration of inorganic metals in the emission aerosol. Both A549 cells and mice exposed to these emissions showed low levels of inflammation but significantly increased genotoxicity. Gaseous emission compounds produced similar genotoxicity and a higher inflammatory response than the corresponding complete combustion emission in A549 cells. Systems biology approaches supported the findings, but we detected differing responses between in vivo and in vitro experiments., Conclusions: Comprehensive in vitro and in vivo exposure studies with emission characterization and systems biology approaches revealed further information on the effects of combustion aerosol toxicity than could be achieved with either method alone. Interestingly, in vitro and in vivo exposures showed the opposite order of the highest DNA damage. In vitro measurements also indicated that the gaseous fraction of emission aerosols may be more important in causing adverse toxicological effects. Combustion aerosols of different wood species result in mild but aerosol specific in vitro and in vivo effects.

Particulate matter is the key to increasing urban air pollution, and research into pollution exposure assessment is an important part of environmental health. In order to classify PM 10 air pollution and to investigate the population exposure to the distribution of PM 10 , daily and monthly PM 10 concentrations of 379 air pollution monitoring stations were obtained for a period from 01/01/2017 to 31/12/2017. Firstly, PM 10 concentrations were classified using the head/tail break clustering algorithm to identify locations with elevated PM 10 levels. Subsequently, population exposure levels were calculated using population-weighted PM 10 concentrations. Finally, the power-law distribution was used to test the distribution of PM 10 polluted areas. Our results indicate that the head/tail break algorithm, with an appropriate segmentation threshold, can effectively identify areas with high PM 10 concentrations. The distribution of the population according to exposure level shows that the majority of people is living in polluted areas. The distribution of heavily PM 10 polluted areas in Germany follows the power-law distribution well, but their boundaries differ from the boundaries of administrative cities; some even cross several administrative cities. These classification results can guide policymakers in dividing the country into several areas for pollution control.

Growing literature has documented varying toxic potencies of source- or site-specific fine particulate matter (PM 2.5 ), as opposed to the practice that treats particle toxicities as independent of composition given the incomplete understanding of the toxicity of the constituents. Quantifying component-specific contribution is the key to unlocking the geographical disparities of particle toxicity from a mixture perspective. In this study, we performed integrated mixture-toxicity experiments and modeling to quantify the contribution of metals and polycyclic aromatic hydrocarbons (PAHs), two default culprit component groups of PM 2.5 toxicity, to in vitro oxidative stress caused by wintertime PM 2.5 from Beijing and Guangzhou, two megacities in China. PM 2.5 from Beijing exhibited greater toxic potencies at equal mass concentrations. The targeted chemical analysis revealed higher burden of metals and PAHs per unit mass of PM 2.5 in Beijing. These chemicals together explained 38 and 24% on average of PM 2.5 -induced reactive oxygen species in Beijing and Guangzhou, respectively, while >60% of the effects remained to be resolved in terms of contributing chemicals. PAHs contributed approximately twice the share of the PM 2.5 mixture effects as metals. Fe, Cu, and Mn were the dominant metals, constituting >80% of the metal-shared proportion of the PM 2.5 effects. Dibenzo[ a, l]pyrene alone explained >65% of the PAH-shared proportion of the PM 2.5 toxicity effects. The significant contribution from coal combustion and vehicular emissions in Beijing suggested the major source disparities of toxicologically active PAHs between the two cities. Our study provided novel quantitative insights into the role of varying toxic component profiles in shaping the differential toxic potencies of city-specific PM 2.5 pollution.

Residential wood combustion (RWC) emits high amounts of volatile organic compounds (VOCs) into ambient air, leading to formation of secondary organic aerosol (SOA), and various health and climate effects. In this study, the emission factors of VOCs from a logwood-fired modern masonry heater were measured using a Proton-Transfer-Reactor Time-of-Flight Mass Spectrometer. Next, the VOCs were aged in a 29 m 3 Teflon chamber equipped with UV black lights, where dark and photochemical atmospheric conditions were simulated. The main constituents of the VOC emissions were carbonyls and aromatic compounds, which accounted for 50%-52% and 30%-46% of the detected VOC emission, respectively. Emissions were highly susceptible to different combustion conditions, which caused a 2.4-fold variation in emission factors. The overall VOC concentrations declined considerably during both dark and photochemical aging, with simultaneous increase in particulate organic aerosol mass. Especially furanoic and phenolic compounds decreased, and they are suggested to be the major precursors of RWC-originated SOA in all aging conditions. On the other hand, dark aging produced relatively high amounts of nitrogen-containing organic compounds in both gas and particulate phase, while photochemical aging increased especially the concentrations of certain gaseous carbonyls, particularly acid anhydrides.

During many measurements it is important to account for possible changes in the gas-particle distribution of aerosols containing semi-volatile organic compounds (SVOCs). If denuders are combined with currently used personal air samplers, a simultaneous differential sampling of the gas and particle phase is possible. Here we analysed the transmission efficiency of denuders based on multi-channel silicone rubber traps (setup: 9 cm long glass liner (ID 4 mm), containing 22 parallel silicone rubber tubes (55 mm long, ID 0.3 mm, OD 0.5 mm)) with polystyrene latex (PSL) particles for different scenarios. n-Hexadecane, dimethyl phthalate and diethylene glycol gases were used to measure the time-dependent gas phase collection efficiency of a denuder. Additionally, the evaporation of n-hexadecane aerosol particles passing through the denuders was investigated. Our results showed high transmission efficiencies from 91 to 100% (variation coefficients 3.69-9.65%) for the denuders operated vertically at a flow rate of 0.5 l min -1 . With regard to the gas phase collection efficiency, nonpolar n-hexadecane gas was trapped with higher efficiency (87% after 22 h) than dimethyl phthalate gas (27% after 22 h), while for highly polar diethylene glycol the gas phase collection efficiency was 50% after 2 h. Regarding the evaporation of aerosol particles, smaller particles and lower flow rates led to higher particle volume reduction inside the denuders. In conclusion, the tested denuders are suitable for determining the gas-particle partitioning of SVOC aerosols of nonpolar substances and show above 90% transmission for all tested particle sizes.

Gaseous and particulate emissions from a ship diesel research engine were elaborately analysed by a large assembly of measurement techniques. Applied methods comprised of offline and online approaches, yielding averaged chemical and physical data as well as time-resolved trends of combustion by-products. The engine was driven by two different fuels, a commonly used heavy fuel oil (HFO) and a standardised diesel fuel (DF). It was operated in a standardised cycle with a duration of 2 h. Chemical characterisation of organic species and elements revealed higher concentrations as well as a larger number of detected compounds for HFO operation for both gas phase and particulate matter. A noteworthy exception was the concentration of elemental carbon, which was higher in DF exhaust aerosol. This may prove crucial for the assessment and interpretation of biological response and impact via the exposure of human lung cell cultures, which was carried out in parallel to this study. Offline and online data hinted at the fact that most organic species in the aerosol are transferred from the fuel as unburned material. This is especially distinctive at low power operation of HFO, where low volatility structures are converted to the particulate phase. The results of this study give rise to the conclusion that a mere switching to sulphur-free fuel is not sufficient as remediation measure to reduce health and environmental effects of ship emissions.

Open biomass burning from wildfires and the prescribed burning of forests and farmland is a frequent occurrence in South-East Queensland (SEQ), Australia. This work reports on data collected from 10 to 30 September 2011, which covers the days before (10-14 September), during (15-20 September) and after (21-30 September) a period of biomass burning in SEQ. The aim of this project was to comprehensively quantify the impact of the biomass burning on air quality in Brisbane, the capital city of Queensland. A multi-parameter field measurement campaign was conducted and ambient air quality data from 13 monitoring stations across SEQ were analysed. During the burning period, the average concentrations of all measured pollutants increased (from 20% to 430%) compared to the non-burning period (both before and after burning), except for total xylenes. The average concentration of O3, NO2, SO2, benzene, formaldehyde, PM10, PM2.5 and visibility-reducing particles reached their highest levels for the year, which were up to 10 times higher than annual average levels, while PM10, PM2.5 and SO2 concentrations exceeded the WHO 24-hour guidelines and O3 concentration exceeded the WHO maximum 8-hour average threshold during the burning period. Overall spatial variations showed that all measured pollutants, with the exception of O3, were closer to spatial homogeneity during the burning compared to the non-burning period. In addition to the above, elevated concentrations of three biomass burning organic tracers (levoglucosan, mannosan and galactosan), together with the amount of non-refractory organic particles (PM1) and the average value of f60 (attributed to levoglucosan), reinforce that elevated pollutant concentration levels were due to emissions from open biomass burning events, 70% of which were prescribed burning events. This study, which is the first and most comprehensive of its kind in Australia, provides quantitative evidence of the significant impact of open biomass burning events, especially prescribed burning, on urban air quality. The current results provide a solid platform for more detailed health and modelling investigations in the future., (Copyright © 2016 Elsevier Ltd. All rights reserved.)

To achieve unattended continuous long-term (eg., 1 week) sampling of size-segregated 24-h ambient particulate matter (PM), a sampling strategy of a modified 3-stage rotating drum impactor (RDI) in series with a sequential filter sampler was introduced and verified in a field campaign. Before the field sampling, lab experiment was conducted to test the collection efficiency of the third stage of the RDI using the quartz-fiber filter (QFF) as the substrate. The measured value is 0.36 μm, which is larger than the nominal value 0.1 μm. A fast direct analysis of organic species in all size fractions (<0.36, 0.36-1, 1-2.4, and 2.4-10 μm) of 24-h ambient samples was done using in situ derivatization thermal desorption gas chromatography time-of-flight mass spectrometry (IDTD-GC-TOFMS). A few secondary originated polar markers (dicarboxylic acids, cis-pinonic acid, etc.) were introduced and evaluated using this method for the first time and quantified simultaneously with polycyclic aromatic hydrocarbons (PAH) in the filter samples (<0.36 μm). For the other RDI strip samples (0.36-1, 1-2.4, and 2.4-10 μm), PAH and levoglucosan were quantified. The comparability of two such sampler sets was verified with respect to the PM collection profile of the two RDIs as well as measured concentration of chemical compounds in each sampled size fraction, so that a future epidemiological study on the relationship between the finest PM/its chemical composition and health outcome could be carried out through parallel sampling at two sites. The internal correlations between the size-segregated organic compounds are discussed. Besides, the correlations between the size-segregated organic species and size-segregated particulate number concentration (PNC) as well as meteorological parameter are discussed as well.

Rapid industrialization and urbanization in developing countries has led to an increase in air pollution, along a similar trajectory to that previously experienced by the developed nations. In China, particulate pollution is a serious environmental problem that is influencing air quality, regional and global climates, and human health. In response to the extremely severe and persistent haze pollution experienced by about 800 million people during the first quarter of 2013 (refs 4, 5), the Chinese State Council announced its aim to reduce concentrations of PM2.5 (particulate matter with an aerodynamic diameter less than 2.5 micrometres) by up to 25 per cent relative to 2012 levels by 2017 (ref. 6). Such efforts however require elucidation of the factors governing the abundance and composition of PM2.5, which remain poorly constrained in China. Here we combine a comprehensive set of novel and state-of-the-art offline analytical approaches and statistical techniques to investigate the chemical nature and sources of particulate matter at urban locations in Beijing, Shanghai, Guangzhou and Xi'an during January 2013. We find that the severe haze pollution event was driven to a large extent by secondary aerosol formation, which contributed 30-77 per cent and 44-71 per cent (average for all four cities) of PM2.5 and of organic aerosol, respectively. On average, the contribution of secondary organic aerosol (SOA) and secondary inorganic aerosol (SIA) are found to be of similar importance (SOA/SIA ratios range from 0.6 to 1.4). Our results suggest that, in addition to mitigating primary particulate emissions, reducing the emissions of secondary aerosol precursors from, for example, fossil fuel combustion and biomass burning is likely to be important for controlling China's PM2.5 levels and for reducing the environmental, economic and health impacts resulting from particulate pollution.

Children are particularly susceptible to air pollution and schools are examples of urban microenvironments that can account for a large portion of children's exposure to airborne particles. Thus this paper aimed to determine the sources of primary airborne particles that children are exposed to at school by analyzing selected organic molecular markers at 11 urban schools in Brisbane, Australia. Positive matrix factorization analysis identified four sources at the schools: vehicle emissions, biomass burning, meat cooking and plant wax emissions accounting for 45%, 29%, 16% and 7%, of the organic carbon respectively. Biomass burning peaked in winter due to prescribed burning of bushland around Brisbane. Overall, the results indicated that both local (traffic) and regional (biomass burning) sources of primary organic aerosols influence the levels of ambient particles that children are exposed at the schools. These results have implications for potential control strategies for mitigating exposure at schools., (Copyright © 2014 Elsevier Ltd. All rights reserved.)

Direct thermal desorption and in-situ derivatization thermal desorption methods in conjunction with gas chromatography time-of-flight mass spectrometry have been characterized and evaluated for analysis of trace components from filters loaded with ambient particulate matter (PM). The limits of quantification were in the range of 7-24 pg for n-alkanes, 20 pg for hopanes, and 4-22 pg for polycyclic aromatic hydrocarbons (PAH). The limit of quantification was defined as the minimum amount of substance that conforms to the minimum distinguishable signal plus 9 times the standard deviation of this background signal from PM-loaded filters. The method has been successfully applied to low-volume samples from ambient PM collected with stationary and personal samplers. Stationary samples were collected in winter 2008 and 2010 in Augsburg, Germany. Sample aliquots of 0.2-0.3 m³ from stationary sampling were analyzed. High diurnal variation in concentration and source contribution was found especially during periods with low wind speed and low mixing layer height. High contributions of solid fuel combustion (wood and coal) were found in evening and nighttime samples, leading to peak PAH concentrations at midnight more than 10 times higher than at noon. Finally, the method was applied to samples collected by means of a personal sampler, i.e. a micro aethalometer, in Xi'an, China. Quantitative data on n-alkanes, hopanes, and PAH were obtained from sample volumes of 17 and 24 l. The impact of different sources such as vehicular and biogenic emissions could be distinguished.

The on-line analysis of single aerosol particles with mass spectrometrical methods is an important tool for the investigation of aerosols. Often, a single laser pulse is used for one-step laser desorption/ionisation of aerosol particles. Resulting ions are detected with time-of-flight mass spectrometry. With this method, the detection of inorganic compounds is possible. The detection of more fragile organic compounds and carbon clusters can be accomplished by separating the desorption and the ionisation in two steps, e.g. by using two laser pulses. A further method is, using a heated metal surface for thermal desorption of aerosol particles. If an ultraviolet laser is used for ionisation, a selective ionisation of polycyclic aromatic hydrocarbons (PAH) and alkylated PAH is possible via a resonance-enhanced multiphoton-ionisation process. Laser velocimetry allows individual laser triggering for single particles and additionally delivers information on aerodynamic particle diameters. It was shown that particles deriving from different combustion sources can be differentiated according to their PAH patterns. For example, retene, a C(4)-alkylated phenanthrene derivative, is a marker for the combustion of coniferous wood. In this paper, the first field application of a thermal desorption resonance-enhanced multiphoton-ionisation single particle time-of-flight mass spectrometer during a measurement campaign in Augsburg, Germany in winter 2010 is presented. Larger PAH-containing particles (i.e. with aerodynamic diameters larger than 1 μm), which are suspected to be originated by re-suspension processes of agglomerated material, were in the focus of the investigation. Due to the low concentration of these particles, an on-line virtual impactor enrichment system was used. The detection of particle-bound PAH in ambient particles in this larger size region was possible and in addition, retene could be detected on several particles, which allows to identify wood combustion as generic source of these particles. The observed diurnal distribution of these larger particles, however, support the origin by traffic induced re-suspension of sedimented/agglomerated material.

This study reports a general assessment of the organic composition of the PM(2.5) samples collected in the city of Augsburg, Germany in a summer (August-September 2007) and a winter (February-March 2008) campaign of 36 and 30 days, respectively. The samples were directly submitted to in-situ derivatisation thermal desorption gas chromatography coupled with time of flight mass spectrometry (IDTD-GC-TOFMS) to simultaneously determine the concentrations of many classes of molecular markers, such as n-alkanes, iso- and anteiso-alkanes, polycyclic aromatic hydrocarbons (PAHs), oxidized PAHs, n-alkanoic acids, alcohols, saccharides and others. The PCA analysis of the data identified the contributions of three emission sources, i.e., combustion sources, including fossil fuel emissions and biomass burning, vegetative detritus, and oxidized PAHs. The PM chemical composition shows seasonal trend: winter is characterized by high contribution of petroleum/wood combustion while the vegetative component and atmospheric photochemical reactions are predominant in the hot season., (Copyright © 2011 Elsevier Ltd. All rights reserved.)

Context: The aerosol components responsible for the adverse health effects of the exposure to particulate matter (PM) have not been conclusively identified, and there is especially little information on the role of particulate organic compounds (POC)., Objective: This study evaluated the role of PM and POC with regard to daily symptoms., Methods: One hundred and fifty-three myocardial infarction survivors from Augsburg, Germany, recorded daily occurrence of different symptoms in winter 2003/2004. Ambient concentrations of PM with a diameter <2.5 μm (PM(2.5)), particle number concentration (PNC), PM(2.5)-bound hopanes, and polycyclic aromatic hydrocarbons (PAH) were quantified. Data were analyzed using generalized estimating equations adjusting for meteorological and other time-variant confounders., Results: The odds for avoidance of physically demanding activities due to heart problems increased immediately associated with most POC measures (e.g. 5% per 1.08 ng/m(3) increase in benzo[a]pyrene, 95%-confidence interval (CI):1-9%) and tended to a delayed decrease. After a 2-day delayed decrease associated with hopanes, the odds for shortness of breath increased consistently after 3 days with almost all POC measures (e.g. 4% per 0.21 ng/m(3) increase in 17α(H), 21β(H)-hopane, CI: 1-8%). The odds for heart palpitations marginally increased immediately in association with PNC (8% per 8146 cm(-3) increase in PNC, CI: 0-16%)., Conclusions: The study showed an association between PM, particle-bound POC, and daily symptoms. The organic compounds may be causally related with cardiovascular health or act rather as indicators for traffic- and combustion-related particles.

Several epidemiological studies have shown that in the human population ambient particulate matter (PM) is associated with adverse health effects. Little is known, however, about the relative effects of aerosol constituents. Since 2002, diurnal samples of ambient PM2.5 were analysed by automated methods for the quantification of particle-associated organic compounds (POC). Data on chemical composition have been investigated in epidemiological and biological effect studies. As a result of these studies, the associations found between PAH concentration and symptoms of myocardial infarction survivors suggest a major influence of combustion sources on cardiovascular health effects. The correlations found between formation of reactive oxygen species and the presence of specific organic compounds suggests an important influence of biomass combustion particles in PM2.5-associated oxidative stress.

PM2.5 filter samples were collected in summer 2005 at an urban background site in Augsburg, Germany. They were analyzed for polycyclic aromatic hydrocarbons (PAH) and their oxygenated derivatives (O-PAH) using gas chromatography/mass spectrometry. Oxygen free radical formation (reactive oxygen substances, ROS) was measured by electron spin resonance (ESR) spectroscopy after addition of spin trapping agent directly on the same filters. The concentrations of ambient, high-boiling PAH and O-PAH were highly correlated to ROS formation, even better than to particulate mass or number concentration. Correlations were most pronounced for some polycyclic aromatic monoketones (e.g., benz[de]anthracene-7-one), which are not yet reported in literature to be redox cycling active. The association found between ESR measurements and the presence of specific semivolatile organic compounds suggests an important influence of wood burning in PM2.5-associated ROS formation. These results indicate that further research on the relationship between radical formation and presence of specific O-PAH and semivolatile organic compounds (SVOC) are likely to provide a better understanding of the relationship between the source-dependent chemical composition of PM and the toxicological risks associated with PM exposure.

Concentrations of ambient semivolatile organic compounds (SVOC) in the PM2.5 fraction of Augsburg, Germany, have been monitored on a daily basis from January 2003 through December 2004. Samples were taken in a large garden in the city center. Quantitative analysis of n-alkanes, alkanones, alkanoic acid methylesters, long chain linear alkyl benzenes and toluenes, hopanes, polycyclic aromatic hydrocarbons (PAH) and oxidized PAH, and some abietan type diterpenes was done. All compounds showed distinct seasonal variations in concentration. Most compounds showed highest concentrations during the cold seasons, but some n-alkanones and 6,10,14-trimethylpentadecanone showed maximum concentration during summer. Changes in patterns between and within compound classes were obvious, e.g., the hopane pattern exhibited a strong seasonal variation. The main source related contributions to changes observed were discussed. Using positive matrix factorization (PMF) for the statistical investigation of the data set, five factors have been separated. These factors are dominated by the pattern of single sources or groups of similar sources: factor 1, lubricating oil; factor 2, emissions of unburned diesel and heating oil consumption; factor 3, wood combustion; factor 4, brown coal combustion; and factor 5, biogenic emissions and transport components. Like the SVOC, the factors showed strong seasonality with highest values in winter for factors 1-4 and in summer for factor 5.

Urban aerosol was collected in a summer and a winter campaign for 7 and 3 days, respectively. Low volume samples were taken with a time resolution of 160 min using a filter/sorption cartridge system extended by an ozone scrubber. Concentrations of mainly particle associated polycyclic aromatic hydrocarbons (PAH) and oxidised PAH (O-PAH) were determined by gas chromatography/high resolution mass spectrometry. The sampling site was located in the city centre of Augsburg, Germany, near major roads with high traffic volume. The daily concentrations and profiles were mainly governed by local emissions from traffic and domestic heating, as well as by the meteorological conditions. During the winter campaign, concentrations were more than 10 fold higher than during the summer campaign. Highest concentrations were found concurrent with low boundary layer heights and low wind speeds. Significant diurnal variation of the PAH profiles was observed. Enhanced influences of traffic related PAH on the PAH profiles were evident during daytime in summer, whereas emissions from hot water generation and domestic heating were obvious during the night time of both seasons. A general idea about the global meteorological situation was acquired using back trajectory calculations (NOAA ARL HYSPLIT4). Due to high local emissions in combination with low air exchange during the two sampling campaigns, effects of mesoscale transport were not clearly observable.

Studies on health effects of air pollutants ideally define exposure through the collection of air samples in the participants' homes. Concentrations derived from these samples are then considered as an estimate for the average concentration of air pollutants in the homes. Conclusions drawn from such studies therefore depend very much on the validity of the measured air pollution concentrations. In this paper we analysed repeated BTEX and NO(2) measurements with a time period of several months lying between the two conducted home visits. We investigated the variability of their concentrations over time by determining correlation coefficients and calculating within- and between-home variances. Our population consisted of 631 homes of participants from two cohort studies within the framework of the German study on Indoor Factors and Genetics in Asthma. Air pollutants were measured using passive samplers both indoors and outdoors. The measured BTEX concentrations were poorly correlated, with Pearson's correlation coefficient r ranging from -0.19 to 0.27. Additionally, a considerable seasonal effect could be observed. A higher correlation was found for the NO(2) concentrations with r ranging between 0.24 and 0.55. For the BTEX, the between-home variance was bigger than the within-home variance, for NO(2) both variances were of about the same order. Our results indicate that in a setting of moderate climate like in Germany, the variability of BTEX and NO(2) concentrations over time is high and a single measurement is a poor surrogate for the long-term concentrations of these air pollutants.

• OMICs analysis reveals a strong impact of the gas phase of wood smoke. • CMAP indicates DPC agents as drivers of OMICs response. • Carbonyls were identified as DPC agents and key pollutants triggering DNA damage and stress signalling. Epidemiological studies identified air pollution as one of the prime causes for human morbidity and mortality, due to harmful effects mainly on the cardiovascular and respiratory systems. Damage to the lung leads to several severe diseases such as fibrosis, chronic obstructive pulmonary disease and cancer. Noxious environmental aerosols are comprised of a gas and particulate phase representing highly complex chemical mixtures composed of myriads of compounds. Although some critical pollutants, foremost particulate matter (PM), could be linked to adverse health effects, a comprehensive understanding of relevant biological mechanisms and detrimental aerosol constituents is still lacking. Here, we employed a systems toxicology approach focusing on wood combustion, an important source for air pollution, and demonstrate a key role of the gas phase, specifically carbonyls, in driving adverse effects. Transcriptional profiling and biochemical analysis of human lung cells exposed at the air–liquid-interface determined DNA damage and stress response, as well as perturbation of cellular metabolism, as major key events. Connectivity mapping revealed a high similarity of gene expression signatures induced by wood smoke and agents prompting DNA-protein crosslinks (DPCs). Indeed, various gaseous aldehydes were detected in wood smoke, which promote DPCs, initiate similar genomic responses and are responsible for DNA damage provoked by wood smoke. Hence, systems toxicology enables the discovery of critical constituents of complex mixtures i.e. aerosols and highlights the role of carbonyls on top of particulate matter as an important health hazard. [ABSTRACT FROM AUTHOR]