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It is being suggested that particle-bound or particle-induced reactive oxygen species (ROS), which significantly contribute to the oxidative potential (OP) of aerosol particles, are a promising metric linking aerosol compositions to toxicity and adverse health effects. However, accurate ROS quantification remains challenging due to the reactive and short-lived nature of many ROS components and the lack of appropriate analytical methods for a reliable quantification. Consequently, it remains difficult to gauge their impact on human health, especially to identify how aerosol particle sources and atmospheric processes drive particle-bound ROS formation in a real-world urban environment. In this study, using a novel online particle-bound ROS instrument (OPROSI), we comprehensively characterized and compared the formation of ROS in secondary organic aerosols (SOAs) generated from organic compounds that represent anthropogenic (naphthalene, SOANAP) and biogenic (β-pinene, SOAβPIN) precursors. The SOA mass was condensed onto soot particles (SP) under varied atmospherically relevant conditions (photochemical aging and humidity) to mimic the SOA formation from a mixing of traffic-related carbonaceous primary aerosols and volatile organic compounds (VOCs). We systematically analyzed the ability of the aqueous extracts of the two aerosol types (SOANAP-SP and SOAβPIN-SP) to induce ROS production and OP. We further investigated cytotoxicity and cellular ROS production after exposing human lung epithelial cell cultures (A549) to extracts of the two aerosols. A significant finding of this study is that more than 90 % of all ROS components in both SOA types have a short lifetime, highlighting the need to develop online instruments for a meaningful quantification of ROS. Our results also show that photochemical aging promotes particle-bound ROS production and enhances the OP of the aerosols. Compared to SOAβPIN-SP, SOANAP-SP elicited a higher acellular and cellular ROS production, a higher OP, and a lower cell viability. These consistent results between chemical-based and biological-based analyses indicate that particle-bound ROS quantification could be a feasible metric to predict aerosol particle toxicity and adverse human effects. Moreover, the cellular ROS production caused by SOA exposure not only depends on aerosol type but is also affected by exposure dose, highlighting a need to mimic the process of particle deposition onto lung cells and their interactions as realistically as possible to avoid unknown biases.

We investigated concentrations of organic carbon (OC), elemental carbon (EC), and a wide range of particle-bound organic compounds in daily sampled PM2.5 at the remote Pha Din (PDI) – Global Atmosphere Watch (GAW) monitoring station in northwestern Vietnam during an intense 3-week sampling campaign from 23 March to 12 April 2015. The site is known to receive trans-regional air masses during large-scale biomass burning (BB) episodes. BB is a globally widespread phenomenon and BB emission characterization is of high scientific and societal relevance. Emissions composition is influenced by multiple factors (e.g., fuel and thereby vegetation type, fuel moisture, fire temperature, available oxygen). Due to regional variations in these parameters, studies in different world regions are needed. OC composition provides valuable information regarding the health- and climate-relevant properties of PM2.5. Yet, OC composition studies from PDI are missing in the scientific literature to date. Therefore, we quantified 51 organic compounds simultaneously by in situ derivatization thermal desorption gas chromatography and time-of-flight mass spectrometry (IDTD-GC-TOFMS). Anhydrosugars, methoxyphenols, n-alkanes, fatty acids, polycyclic aromatic hydrocarbons, oxygenated polycyclic aromatic hydrocarbons, nitrophenols, and OC were used in a hierarchical cluster analysis highlighting distinctive patterns for periods under low, medium, and high BB influence. The highest particle phase concentration of the typical primary organic aerosol (POA) and possible secondary organic aerosol (SOA) constituents, especially nitrophenols, were found on 5 and 6 April. We linked the trace gas mixing ratios of methane (CH4), carbon dioxide (CO2), carbon monoxide (CO), and ozone (O3) to the statistical classification of BB events based on OA composition and found increased CO and O3 levels during medium and high BB influence. Likewise, a backward trajectory analysis indicates different source regions for the identified periods based on the OA clusters, with cleaner air masses arriving from the northeast, i.e., mainland China and the Yellow Sea. The more polluted periods are characterized by trajectories from the southwest, with more continental recirculation of the medium cluster and more westerly advection for the high cluster. These findings highlight that BB activities in northern Southeast Asia significantly enhance the regional organic aerosol loading and also affect the carbonaceous PM2.5 constituents and the trace gases in northwestern Vietnam. The presented analysis adds valuable data on the carbonaceous and chemical composition of PM2.5, in particular of OC, in a region of scarce data availability, and thus offers a reference dataset from Southeast Asian large-scale BB for future studies. Such a reference dataset may be useful for the evaluation of atmospheric transport simulation models, or for comparison with other world regions and BB types, such as Australian bush fires, African savannah fires, or tropical peatland fires.

Residential wood combustion (RWC) emits large amounts of gaseous and particulate organic aerosol (OA). In the atmosphere, the emission is transformed via oxidative reactions, which are under daylight conditions driven mainly by hydroxyl radicals (OH). This continuing oxidative ageing produces secondary OA and may change the health- and climate-related properties of the emission. However, it is not well known how the composition of RWC-originated OA changes as the function of OH exposure. In this work, emissions from two modern residential logwood combustion appliances were photochemically aged in an oxidation flow reactor (OFR) with various OH exposure levels, reaching up to 6×1011 s cm−3 (equivalent to 1 week in the atmosphere). Gaseous organic compounds were analysed by proton transfer reaction time-of-flight mass spectrometry (PTR-ToF-MS), while particulate OA was analysed online by a high-resolution soot particle aerosol mass spectrometer (SP-HR-ToF-AMS) and offline by in situ derivatization thermal desorption–gas chromatography–time-of-flight mass spectrometry (IDTD-GC-ToF-MS). Photochemical reactions increased the mass of particulate organic carbon by a factor of 1.3–3.9. The increase in mass took place during the first atmospheric equivalent day of ageing, after which the enhancement was independent of the extent of photochemical exposure. However, ageing increased the oxidation state of the particulate OA linearly throughout the assessed range, with ΔH:C/ΔO:C slopes between −0.17 and −0.49 in van Krevelen space. Ageing led to an increase in acidic fragmentation products in both phases, as measured by the IDTD-GC-ToF-MS for the particulate and PTR-ToF-MS for the gaseous phase. For the gaseous organic compounds, the formation of small carbonylic compounds combined with the rapid degradation of primary volatile organic compounds such as aromatic compounds led to a continuous increase in both the O : C and H : C ratios. Overall, the share of polycyclic aromatic compounds (PACs) in particles degraded rapidly during ageing, although some oxygen-substituted PACs, most notably naphthaldehydic acid, increased, in particular during relatively short exposures. Similarly, the concentrations of particulate nitrophenols rose extensively during the first atmospheric equivalent day. During continuous photochemical ageing, the dominant transformation mechanisms shifted from the initial gas-phase functionalization/condensation to the transformation of the particulate OA by further oxidation reactions and fragmentation. The observed continuous transformation of OA composition throughout a broad range of OH exposures indicates that the entire atmospheric lifetime of the emission needs to be explored to fully assess the potential climate and health effects of RWC emissions.

Residential wood burning contributes to the total atmospheric aerosol burden; however, large uncertainties remain in the magnitude and characteristics of wood burning products. Primary emissions are influenced by a variety of parameters, including appliance type, burner wood load and wood type. In addition to directly emitted particles, previous laboratory studies have shown that oxidation of gas-phase emissions produces compounds with sufficiently low volatility to readily partition to the particles, forming considerable quantities of secondary organic aerosol (SOA). However, relatively little is known about wood burning SOA, and the effects of burn parameters on SOA formation and composition are yet to be determined. There is clearly a need for further study of primary and secondary wood combustion aerosols to advance our knowledge of atmospheric aerosols and their impacts on health, air quality and climate. For the first time, smog chamber experiments were conducted to investigate the effects of wood loading on both primary and secondary wood combustion products. Products were characterized using a range of particle- and gas-phase instrumentation, including an aerosol mass spectrometer (AMS). A novel approach for polycyclic aromatic hydrocarbon (PAH) quantification from AMS data was developed and results were compared to those from GC-MS analysis of filter samples. Similar total particle mass emission factors were observed under high and average wood loadings; however, high fuel loadings were found to generate significantly higher contributions of PAHs to the total organic aerosol (OA) mass compared to average loadings. PAHs contributed 15 ± 4% (mean ±2 sample standard deviations) to the total OA mass in high-load experiments, compared to 4 ± 1% in average-load experiments. With aging, total OA concentrations increased by a factor of 3 ± 1 for high load experiments compared to 1.6 ± 0.4 for average-load experiments. In the AMS, an increase in PAH and aromatic signature ions at lower m / z values, likely fragments from larger functionalized PAHs, was observed with aging. Filter samples also showed an increase in functionalized PAHs in the particles with aging, particularly oxidized naphthalene species. As PAHs and their oxidation products are known to have deleterious effects on health, this is a noteworthy finding to aid in the mitigation of negative wood burning impacts by improving burner operation protocols.

The impact of wood combustion on ambient aerosols was investigated in Augsburg, Germany during a winter measurement campaign of a six-week period. Special attention was paid to the high time resolution observations of wood combustion with different mass spectrometric methods. Here we present and compare the results from an Aerodyne aerosol mass spectrometer (AMS) and gas chromatographic – mass spectrometric (GC-MS) analysed PM1 filters on an hourly basis. This includes source apportionment of the AMS derived organic matter (OM) using positive matrix factorisation (PMF) and analysis of levoglucosan as wood combustion marker, respectively. During the measurement period nitrate and OM mass are the main contributors to the defined submicron particle mass of AMS and Aethalometer with 28% and 35%, respectively. Wood combustion organic aerosol (WCOA) contributes to OM with 23% on average and 27% in the evening and night time. Conclusively, wood combustion has a strong influence on the organic matter and overall aerosol composition. Levoglucosan accounts for 14% of WCOA mass with a higher percentage in comparison to other studies. The ratio between the mass of levoglucosan and organic carbon amounts to 0.06. This study is unique in that it provides a one-hour time resolution comparison between the wood combustion results of the AMS and the GC-MS analysed filter method at a PM1 particle size range. The comparison of the concentration variation with time of the PMF WCOA factor, levoglucosan estimated by the AMS data and the levoglucosan measured by GC-MS is highly correlated (R2 = 0.84), and a detailed discussion on the contributors to the wood combustion marker ion at mass-to-charge ratio 60 is given. At the end, both estimations, the WCOA factor and the levoglucosan concentration estimated by AMS data, allow to observe the variation with time of wood combustion emissions (gradient correlation with GC-MS levoglucosan of R2 = 0.84). In the case of WCOA, it provides the estimated magnitude of wood combustion emission. Quantitative estimation of the levoglucosan concentration from the AMS data is problematic due to its overestimation in comparison to the levoglucosan measured by the GC-MS.

An in-situ derivatization thermal desorption method followed by gas chromatography and time-of-flight mass spectrometry (IDTD-GC-TOFMS) was developed for determination of polar organic compounds together with non-polar compounds in one measurement. Hydroxyl and carboxyl groups of compounds such as anhydrous sugars, alcohols and phenols, fatty acids and resin acids are targets of the derivatization procedure. Derivatization is based on silylation with N-Methyl-N-trimethylsilyl-trifluoroacetamide (MSTFA) during the step of thermal desorption. The high temperature of 300 °C during desorption is utilized for the in-situ derivatization on the collection substrate (quartz fibre filters) accelerating the reaction rate. Thereby, the analysis time is as short as without derivatization. At first the filter surface is dampened with derivatization reagent before insertion of the sample into the thermal desorption unit. To ensure ongoing derivatization during thermal desorption the carrier gas is enriched with MSTFA until the desorption procedure is finished. The precisions of all studied analytes were below 17 % within a calibration range from 22 pg (abietic acid) up to 342 ng (levoglucosan). Limits of quantification (LOQ) for polycyclic aromatic hydrocarbons (PAH) were between 1 pg (fluoranthene) and 8 pg (indeno[1,2,3-cd]pyrene), for resin acids 37–102 pg and for studied phenols 4–144 pg. LOQ for levoglucosan was 17 pg.

Emissions from road traffic and residential heating contribute to urban air pollution. Advances in emission reduction technologies may alter the composition of emissions and affect their fate during atmospheric processing. Here, emissions of a gasoline car and a wood stove, both equipped with modern emission mitigation technology, were photochemically aged in an oxidation flow reactor to the equivalent of one to five days of photochemical aging. Fresh and aged exhausts were analyzed by ultrahigh resolution mass spectrometry. The gasoline car equipped with a three-way catalyst and a gasoline particle filter emitted minor primary fine particulate matter (PM2.5), but aging led to formation of particulate low-volatile, oxygenated and highly nitrogen-containing compounds, formed from volatile organic compounds (VOCs) and gases incl. NO x , SO 2 , and NH 3 . Reduction of the particle concentration was also observed for the application of an electrostatic precipitator with residential wood combustion but with no significant effect on the chemical composition of PM2.5. Comparing the effect of short and medium photochemical exposures on PM2.5 of both emission sources indicates a similar trend for formation of new organic compounds with increased carbon oxidation state and nitrogen content. The overall bulk compositions of the studied emission exhausts became more similar by aging, with many newly formed elemental compositions being shared. However, the presence of particulate matter in wood combustion results in differences in the molecular properties of secondary particles, as some compounds were preserved during aging.

Agricultural fires are a major source of biomass-burning organic aerosols (BBOAs) with impacts on health, the environment, and climate. In this study, globally relevant BBOA emissions from the combustion of sugar cane in both field and laboratory experiments were analyzed using comprehensive two-dimensional gas chromatography time-of-flight mass spectrometry. The derived chemical fingerprints of fresh emissions were evaluated using targeted and nontargeted evaluation approaches. The open-field sugar cane burning experiments revealed the high chemical complexity of combustion emissions, including compounds derived from the pyrolysis of (hemi)cellulose, lignin, and further biomass, such as pyridine and oxime derivatives, methoxyphenols, and methoxybenzenes, as well as triterpenoids. In comparison, laboratory experiments could only partially model the complexity of real combustion events. Our results showed high variability between the conducted field and laboratory experiments, which we, among others, discuss in terms of differences in combustion conditions, fuel composition, and atmospheric processing. We conclude that both field and laboratory studies have their merits and should be applied complementarily. While field studies under real-world conditions are essential to assess the general impact on air quality, climate, and environment, laboratory studies are better suited to investigate specific emissions of different biomass types under controlled conditions., Competing Interests: The authors declare no competing financial interest., (© 2024 The Authors. Published by American Chemical Society.)

Background: The increase in allergies began worldwide with the onset of the Great Acceleration. Environmental pollution and climate change now threaten to cancel out decades of success in health research., Objective: A summary of environmental influences is provided, which not only shows the significant increase in the prevalence of allergies worldwide but also that of noncommunicable diseases. The effects of the climate crisis on allergies and the multifactorial and interfunctional relationships with other environmental changes are described in detail., Material and Methods: In order to obtain an overview of the possible effects of global environmental changes on allergies, a wide range of literature was evaluated and the study results were prepared and summarized., Results: A large number of allergens are influencing the human exposome on a daily basis. These allergens are triggered by environmental changes, such as air pollution in the ambient air and indoors, chemicals in everyday objects or residues in food. People are sensitized by the interaction of allergens and pollutants., Conclusion: The prevalence of allergies is stagnating in industrialized countries. This is probably just the calm before the storm. The accelerating effects of global warming could make pollen and air pollutants even more aggressive in the future. Urgent action is therefore needed to minimize environmental pollution and mitigate climate change., (© 2024. The Author(s), under exclusive licence to Springer Medizin Verlag GmbH, ein Teil von Springer Nature.)

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., 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 The Authors. Published by Elsevier Ltd.. All rights reserved.)

Residential heating with solid fuels is one of the major drivers for poor air quality in Central and Eastern Europe, and coal is still one of the major fuels in countries, such as Poland, the Czech Republic, and Hungary. In this work, emissions from a single-room heater fueled with brown coal briquettes (BCBs) and spruce logs (SLs) were analyzed for signatures of inorganic as well as semivolatile aromatic and low-volatile organic constituents. High variations in organic carbon (OC) emissions of BCB emissions, ranging from 5 to 22 mg MJ -1 , were associated to variations in carbon monoxide (CO) emissions, ranging from 900 to 1900 mg MJ -1 . Residential BCB combustion turned out to be an equally important source of levoglucosan, an established biomass burning marker, as spruce logwood combustion, but showed distinct higher ratios to manosan and galactosan. Signatures of polycyclic aromatic hydrocarbons emitted by BCB combustion exhibited defunctionalization and desubstitution with increasing combustion quality. Lastly, the concept of island and archipelago structural motifs adapted from petroleomics is used to describe the fraction low-volatile organic compounds in particulate emissions, where a transition from archipelago to island motifs in relation with decreasing CO emissions was observed in BCB emissions, while emissions from SL combustion exhibited the island motif.

Biomass burning is a significant anthropogenic source of air pollution, including the preharvest burning of sugar cane. These burn events result in atmospheric emissions, including semivolatile organic compounds, that may have adverse impacts on air quality and human health on a local, regional, and even a global scale. Gaseous and particulate polycyclic aromatic hydrocarbon (PAH) emissions from various sugar cane burn events in the province of Kwa-Zulu Natal in South Africa were simultaneously sampled using a portable denuder sampling technology, consisting of a quartz fiber filter sandwiched between two polydimethylsiloxane multichannel traps. Total gas and particle phase PAH concentrations ranged from 0.05 to 9.85 µg m -3 per individual burn event, and nine PAHs were quantified. Over 85% of all PAHs were found to exist in the gas phase, with smaller two- and three-ring PAHs, primarily naphthalene, 1-methyl naphthalene, and acenaphthylene, being the most dominant and causing the majority of variance between the burn sites. The PAH profiles differed between the different burn events at different sites, emphasizing the significant influence that the crop variety, prevailing weather conditions, and geographical location has on the type and number of pollutants emitted. The potential carcinogenicity of the PAH exposure was estimated based on toxic equivalency factors that showed varying risk potentials per burn event, with the highest value of 5.97 ng m -3 . Environ Toxicol Chem 2023;42:778-792. © 2023 The Authors. Environmental Toxicology and Chemistry published by Wiley Periodicals LLC on behalf of SETAC., (© 2023 The Authors. Environmental Toxicology and Chemistry published by Wiley Periodicals LLC on behalf of SETAC.)

Building demolition following domestic fires or abrasive processing after thermal recycling can release particles harmful for the environment and human health. To mimic such situations, particles release during dry-cutting of construction materials was investigated. A reinforcement material consisting of carbon rods (CR), carbon concrete composite (C³) and thermally treated C³ (ttC³) were physicochemically and toxicologically analyzed in monocultured lung epithelial cells, and co-cultured lung epithelial cells and fibroblasts at the air-liquid interface. C³ particles reduced their diameter to WHO fibre dimensions during thermal treatment. Caused by physical properties or by polycyclic aromatic hydrocarbons and bisphenol A found in the materials, especially the released particles of CR and ttC³ induced an acute inflammatory response and (secondary) DNA damage. Transcriptome analysis indicated that CR and ttC³ particles carried out their toxicity via different mechanisms. While ttC³ affected pro-fibrotic pathways, CR was mostly involved in DNA damage response and in pro-oncogenic signaling., 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 B.V. All rights reserved.)

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.)

The health effects of exposure to secondary organic aerosols (SOAs) are still limited. Here, we investigated and compared the toxicities of soot particles (SP) coated with β-pinene SOA (SOA βPin -SP) and SP coated with naphthalene SOA (SOA Nap -SP) in a human bronchial epithelial cell line (BEAS-2B) residing at the air-liquid interface. SOA βPin -SP mostly contained oxygenated aliphatic compounds from β-pinene photooxidation, whereas SOA Nap -SP contained a significant fraction of oxygenated aromatic products under similar conditions. Following exposure, genome-wide transcriptome responses showed an Nrf2 oxidative stress response, particularly for SOA Nap -SP. Other signaling pathways, such as redox signaling, inflammatory signaling, and the involvement of matrix metalloproteinase, were identified to have a stronger impact following exposure to SOA Nap -SP. SOA Nap -SP also induced a stronger genotoxicity response than that of SOA βPin -SP. This study elucidated the mechanisms that govern SOA toxicity and showed that, compared to SOAs derived from a typical biogenic precursor, SOAs from a typical anthropogenic precursor have higher toxicological potency, which was accompanied with the activation of varied cellular mechanisms, such as aryl hydrocarbon receptor. This can be attributed to the difference in chemical composition; specifically, the aromatic compounds in the naphthalene-derived SOA had higher cytotoxic potential than that of the β-pinene-derived SOA., (Copyright © 2022 The Authors. Published by Elsevier Ltd.. All rights reserved.)

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.

Solid fuel usage in residential heating and cooking is one of the largest sources of ambient and indoor air particulate matter, which causes adverse effects on the health of millions of peoples worldwide. Emissions from solid fuel combustion, such as biomass or coal, are detrimental to health, but toxicological responses are largely unknown. In the present study, we compared the toxicological responses regarding cytotoxicity, inflammation and genotoxicity of spruce (SPR) and brown coal briquette (BCB) combustion aerosols on human alveolar epithelial cells (A549) as well as a coculture of A549 and differentiated human monocytic cells (THP-1) into macrophages exposed at the air-liquid interface (ALI). We included both the high emissions from the first hour and moderate emissions from the third hour of the batch combustion experiment in one ALI system, whereas, in the second ALI system, we exposed the cells during the whole 4-hour combustion experiment, including all combustion phases. Physico-chemical properties of the combustion aerosol were analysed both online and offline. Both SPR and BCB combustion aerosols caused mild cytotoxic but notable genotoxic effects in co-cultured A549 cells after one-hour exposure. Inflammatory response analysis revealed BCB combustion aerosols to cause a mild increase in CXCL1 and CXCL8 levels, but in the case of SPR combustion aerosol, a decrease compared to control was observed., 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 The Authors. Published by Elsevier B.V. All rights reserved.)

Adverse health effects driven by airborne particulate matter (PM) are mainly associated with reactive oxygen species formation, pro-inflammatory effects, and genome instability. Therefore, a better understanding of the underlying mechanisms is needed to evaluate health risks caused by exposure to PM. The aim of this study was to compare the genotoxic effects of two oxidizing agents (menadione and 3-chloro-1,2-propanediol) with three different reference PM (fine dust ERM-CZ100, urban dust SRM1649, and diesel PM SRM2975) on monocytic THP-1 and alveolar epithelial A549 cells. We assessed DNA oxidation by measuring the oxidized derivative 8-hydroxy-2'-deoxyguanosine (8-OHdG) following short and long exposure times to evaluate the persistency of oxidative DNA damage. Cytokinesis-block micronucleus cytome assay was performed to assess chromosomal instability, cytostasis, and cytotoxicity. Particles were characterized by inductively coupled plasma mass spectrometry in terms of selected elemental content, the release of ions in cell medium and the cellular uptake of metals. PM deposition and cellular dose were investigated by a spectrophotometric method on adherent A549 cells. The level of lipid peroxidation was evaluated via malondialdehyde concentration measurement. Despite differences in the tested concentrations, deposition efficiency, and lipid peroxidation levels, all reference PM samples caused oxidative DNA damage to a similar extent as the two oxidizers in terms of magnitude but with different oxidative DNA damage persistence. Diesel SRM2975 were more effective in inducing chromosomal instability with respect to fine and urban dust highlighting the role of polycyclic aromatic hydrocarbons derivatives on chromosomal instability. The persistence of 8-OHdG lesions strongly correlated with different types of chromosomal damage and revealed distinguishing sensitivity of cell types as well as specific features of particles versus oxidizing agent effects. In conclusion, this study revealed that an interplay between DNA oxidation persistence and chromosomal damage is driving particulate matter-induced genome instability., (Copyright © 2022 Elsevier B.V. All rights reserved.)

Anthropogenic air pollution has a severe impact on climate and human health. The immense molecular complexity and diversity of particulate matter (PM) is a result of primary organic aerosol (POA) as well as secondary organic aerosols (SOAs). In this study, a direct inlet probe (DIP), i.e., atmospheric solids analysis probe (ASAP), with ion mobility high-resolution mass spectrometric detection is applied. Primary particulate matter emissions from three sources were investigated. Furthermore, photochemically aged emissions were analyzed. DIP introduction allowed for a direct analysis with almost no sample preparation and resulted in a complex molecular pattern. This pattern shifted through oxidation processes toward heavier species. For diesel emissions, the fuel's chemical characteristic is partially transferred to the particulate matter by incomplete combustion and characteristic alkylated series were found. Polycyclic aromatic hydrocarbons (PAHs) were identified as major contributors. Ion mobility analysis results in drift time profiles used for structural analysis. The apex position was used to prove structural changes, whereas the full-width-at-half-maximum was used to address the isomeric diversity. With this concept, the dominance of one or a few isomers for certain PAHs could be shown. In contrast, a broad isomeric diversity was found for oxygenated species. For the in-depth specification of fresh and aged spruce emissions, the ion mobility resolving power was almost doubled by allowing for three passes in the circular traveling wave design. The results prove that ASAP coupled with ion mobility spectrometry-mass spectrometry (IMS-MS) serves as a promising analytical approach for tackling the vast molecular complexity of PM.

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.

Semi-volatile organic compounds (SVOCs), partitioned between particulates and vapours of an aerosol, require special attention. The toxicological effects caused by the inhalation of such aerosols may depend on the concentration and in which phase the organic compounds are found. A personal denuder-gas-particle separation aerosol sampler was developed to provide information about the partitioning of aerosols from organic compounds. The sampler was tested in a series of controlled laboratory experiments, which confirmed the capability and accuracy of the sampler to measure gas-particle mixtures. An average difference of 14.8 ± 4.8% was found between sampler and reference laboratory instruments. The obtained results showed that our sampler enables a more accurate measurement of the SVOC aerosols' gas-particle fractionation, compared with that of conventional samplers., (© The Author(s) 2020. Published by Oxford University Press on behalf of the British Occupational Hygiene Society.)

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.

Ambient particulate matter (PM) is a leading global environmental health risk. Current air quality regulations are based on airborne mass concentration. However, PM from different sources have distinct chemical compositions and varied toxicity. Connections between emission control measures, air quality, PM composition, and toxicity remain insufficiently elucidated. The current study assessed the composition and toxicity of PM collected in Nanjing, China before, during, and after an air quality intervention for the 2014 Youth Olympic Games. A co-culture model that mimics the alveolar epithelium with the associated macrophages was created using A549 and THP-1 cells. These cells were exposed to size-segregated inhalable PM samples. The composition and toxicity of the PM samples were influenced by several factors including seasonal variation, emission sources, and the air quality intervention. For example, we observed a size-dependent shift in particle mass concentrations during the air quality intervention with an emphasized proportion of smaller particles (PM 2.5 ) present in the air. The roles of industrial and fuel combustion and traffic emissions were magnified during the emission control period. Our analyses revealed that the PM samples demonstrated differential cytotoxic potencies at equal mass concentrations between sampling periods, locations, and time of day, influenced by variations in the predominant emission sources. Coal combustion and industrial emissions were the most important sources affecting the toxicological responses and displayed the least variation in emission contributions between the sampling periods. In conclusion, emission control mitigated cytotoxicity and oxidative stress for particles larger than 0.2 μm, but there was inadequate evidence to determine if it was the key factor reducing the harmful effects of PM 0.2 ., 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.)

The combustion of spruce logwood in a modern residential stove was found to emit polycyclic aromatic hydrocarbons (PAH) and oxygenated polycyclic aromatic hydrocarbons (OPAH) with emission factors of 404 μg MJ -1 of 35 analysed PAH, 317 μg MJ -1 of 11 analysed Oxy-PAH and 12.5 μg MJ -1 of 5 analysed OH-PAH, most of which are known as potential mutagens and carcinogens. Photochemical ageing in an oxidation flow reactor (OFR) degraded particle-bound PAH, which was also reflected in declining PAH toxicity equivalent (PAH-TEQ) values by 45 to 80% per equivalent day of photochemical ageing in the atmosphere. OPAH concentrations decreased less than PAH concentrations during photochemical ageing, supposedly due to their secondary formation, while 1-hydroxynaphthalene, 1,5-dihydroxynaphthalene and 1,8-naphthalaldehydic acid were significantly increased after ageing. Furthermore, secondary organic aerosol (SOA) formation and aromatic compounds not included in targeted analysis were investigated by thermal-optical carbon analysis (TOCA) hyphenate to resonance-enhanced multi-photon ionisation time-of-flight mass spectrometry (REMPI-TOFMS). The commonly used PAH-source indicators phenanthrene/anthracene, fluoranthene/pyrene, retene/chrysene, and indeno[cd]pyrene/benzo[ghi]perylene remained stable during photochemical ageing, enabling identification of wood combustion emissions in ambient air. On the other hand, benz[a]pyrene/benz[e]pyrene and benz[a]anthracene/chrysene were found to decrease with increasing photochemical age. Retene/chrysene was not a proper classifier for the wood combustion emissions of this study, possibly due to more efficient combustion than in open wood burning, from which this diagnostic ratio was initially derived. This study motivates in-depth investigation of degradation kinetics of particle-bound species on different combustion aerosol as well as the consequences of photochemical ageing on toxicity and identification of wood combustion emissions in ambient air., (Copyright © 2019 Elsevier B.V. All rights reserved.)

Industrial processes, coal combustion, biomass burning (BB), and vehicular transport are important sources of atmospheric fine particles (PM 2.5 ) and contribute to ambient air concentrations of health-hazardous species, such as heavy metals, polycyclic aromatic hydrocarbons (PAH), and oxygenated-PAHs (OPAH). In China, emission controls have been implemented to improve air quality during large events, like the Youth Olympic Games (YOG) in August 2014 in Nanjing. In this work, six measurement campaigns between January 2014 and August 2015 were undertaken in Nanjing to determine the effects of emission controls and meteorological factors on PM 2.5 concentration and composition. PAHs, OPAHs, hopanes, n‑alkanes, heavy metals, and several other inorganic elements were measured. PM 2.5 and potassium concentrations were the highest in May-June 2014 indicating the prevalence of BB plumes in Nanjing. Emission controls substantially reduced concentrations of PM 2.5 (31%), total PAHs (59%), OPAHs (37%), and most heavy metals (44-89%) during the YOG compared to August 2015. In addition, regional atmospheric transport and meteorological parameters partly explained the observed differences between the campaigns. The most abundant PAHs and OPAHs were benzo[b,k]fluoranthenes, fluoranthene, pyrene, chrysene, 1,8‑naphthalic anhydride, and 9,10‑anthracenedione in all campaigns. Carbon preference index and the contribution of wax n‑alkanes indicated mainly biogenic sources of n‑alkanes in May-June 2014 and anthropogenic sources in the other campaigns. Hopane indexes pointed to vehicular transport as the major source of hopanes, but contribution of coal combustion was detected in winter 2015. The results provide evidence to the local government of the impacts of the air protection regulations. However, differences between individual components were observed, e.g., concentrations of potentially more harmful OPAHs decreased less than concentrations of PAHs. The results suggest that the proportions of hazardous components in the PM 2.5 may also change considerably due to emission control measures., (Copyright © 2018 Elsevier B.V. All rights reserved.)

Ambient inhalable particulate matter (PM) is a serious health concern worldwide, but especially so in China where high PM concentrations affect huge populations. Atmospheric processes and emission sources cause spatial and temporal variations in PM concentration and chemical composition, but their influence on the toxicological characteristics of PM are still inadequately understood. In this study, we report an extensive chemical and toxicological characterization of size-segregated urban air inhalable PM collected in August and October 2013 from Nanjing, and assess the effects of atmospheric processes and likely emission sources. A549 human alveolar epithelial cells were exposed to day- and nighttime PM samples (25, 75, 150, 200, 300 μg/ml) followed by analyses of cytotoxicity, genotoxicity, cell cycle, and inflammatory response. PM 10-2.5 and PM 0.2 caused the greatest toxicological responses for different endpoints, illustrating that particles with differing size and chemical composition activate distinct toxicological pathways in A549 cells. PM 10-2.5 displayed the greatest oxidative stress and genotoxic responses; both were higher for the August samples compared with October. In contrast, PM 0.2 and PM 2.5-1.0 samples displayed high cytotoxicity and substantially disrupted cell cycle; August samples were more cytotoxic whereas October samples displayed higher cell cycle disruption. Several components associated with combustion, traffic, and industrial emissions displayed strong correlations with these toxicological responses. The lower responses for PM 1.0-0.2 compared to PM 0.2 and PM 2.5-1.0 indicate diminished toxicological effects likely due to aerosol aging and lower proportion of fresh emission particles rich in highly reactive chemical components in the PM 1.0-0.2 fraction. Different emission sources and atmospheric processes caused variations in the chemical composition and toxicological responses between PM fractions, sampling campaigns, and day and night. The results indicate different toxicological pathways for coarse-mode particles compared to the smaller particle fractions with typically higher content of combustion-derived components. The variable responses inside PM fractions demonstrate that differences in chemical composition influence the induced toxicological responses., (Copyright © 2018 The Authors. Published by Elsevier B.V. All rights reserved.)

Denuders are gas-particle partitioning tools and can be used in combination with filters and adsorbers for phase-separated collection of hazardous semi-volatile organic compound (SVOC) aerosols. Here, we investigated the suitability of carbonaceous monolithic multi-channel denuders for this approach. Particle transmission efficiency through the denuders was investigated using particles of polystyrene latex (PSL) and droplets of n-hexadecane and diethylene glycol. The time-dependent vapour collection efficiency was analysed for n-hexadecane and diethylene glycol vapours and also compared to calculated predictions. Our measurements showed an averaged transmission efficiency of 97 ± 4.4% for PSL particles with diameters of 0.51, 0.99, 1.93, and 3.00 µm. Measurements with one denuder and 1.08, 1.98, and 2.97 µm particles consisting of n-hexadecane or diethylene glycol resulted in an averaged transmission efficiency of 99 ± 6.5%. Regarding the vapour collection efficiency at a flow rate of 5 l min-1, n-hexadecane vapour could be adsorbed to a similar extent (91 ± 1.4% for one denuder, 98 ± 0.3% for two denuders) as diethylene glycol vapour (93 ± 1.8% for one denuder, 97 ± 0.9% for two denuders). The comparison between experimental and theoretical vapour collection efficiencies revealed differences around 2.8% for n-hexadecane and around 12.3% for diethylene glycol. The results show that the tested denuders can be used as vapour collection tools for SVOCs, and can be integrated in currently used personal air samplers for separated vapour and particle collection.