Are reactive oxygen species (ROS) a suitable metric to predict toxicity of carbonaceous aerosol particles?

Atmospheric chemistry and physics, Год журнала: 2022, Номер 22(3), С. 1793 - 1809

Опубликована: Фев. 7, 2022

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

Язык: Английский

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Dynamic Wood Smoke Aerosol Toxicity during Oxidative Atmospheric Aging

Environmental Science & Technology, Год журнала: 2023, Номер 57(3), С. 1246 - 1256

Опубликована: Янв. 11, 2023

Wildfires are a major source of biomass burning aerosol to the atmosphere, with their incidence and intensity expected increase in warmer future climate. However, toxicity evolution organic (BBOA) during atmospheric aging remains poorly understood. In this study, we report unique set chemical toxicological metrics BBOA from pine wood smoldering multiphase by gas-phase hydroxyl radicals (OH). Both fresh OH-aged show activity relevant adverse health outcomes. The results two acellular assays (DTT DCFH) significant oxidative potential (OP) reactive oxygen species (ROS) formation BBOA. Also, radical concentrations assessed electron paramagnetic resonance (EPR) spectroscopy increased 50% following heterogeneous aging. This enhancement was accompanied transition predominantly carbon-centered (85%) oxygen-centered (76%) aged aerosols trigger prominent antioxidant defense

Язык: Английский

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Superoxide Formation from Aqueous Reactions of Biogenic Secondary Organic Aerosols

Environmental Science & Technology, Год журнала: 2020, Номер 55(1), С. 260 - 270

Опубликована: Дек. 22, 2020

Reactive oxygen species (ROS) play a central role in aqueous-phase processing and health effects of atmospheric aerosols. Although hydroxyl radical (•OH) hydrogen peroxide (H2O2) are regarded as major oxidants associated with secondary organic aerosols (SOA), the kinetics reaction mechanisms superoxide (O2•–) formation rarely quantified poorly understood. Here, we demonstrate dominant O2•– molar yields 0.01–0.03% from aqueous reactions biogenic SOA generated by •OH photooxidation isoprene, β-pinene, α-terpineol, d-limonene. The temporal evolution is elucidated kinetic modeling cascade including decomposition hydroperoxides, oxidation primary or alcohols, unimolecular α-hydroxyperoxyl radicals. Relative various types ROS reflect relative abundance hydroperoxides alcohols contained SOA. These findings mechanistic understanding have important implications on fate particle-phase highly oxygenated molecules well oxidative stress upon respiratory deposition.

Язык: Английский

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Environmentally Persistent Free Radicals, Reactive Oxygen Species Generation, and Oxidative Potential of Highway PM_2.5

ACS Earth and Space Chemistry, Год журнала: 2021, Номер 5(8), С. 1865 - 1875

Опубликована: Июль 9, 2021

In urban environments, vehicle exhaust and nonexhaust emissions represent important sources of fine particulate matter with an aerodynamic diameter less than 2.5 μm (PM2.5), which plays a central role in adverse health effects oxidative stress. We collected PM2.5 filter samples from two highway sites (Anaheim Long Beach, CA) site (Irvine, to quantify environmentally persistent free radicals (EPFRs) contained the generation radical forms reactive oxygen species (ROS) water using electron paramagnetic resonance spectroscopy. The EPFR concentrations were 36 ± 14 pmol m–3 at sites, about times higher those site. EPFRs correlate positively well CO, NOx, elemental organic carbon, indicating that are emitted vehicular exhaust. Good correlations Fe Cu may indicate stabilized by tire brake wears. negatively correlated ozone, suggesting photochemistry does not play large formation possibly also quenched ozone. Highway found generate mainly OH aqueous phase. generated ROS mass show good correlation EPFRs, implying generation. potentials as quantified dithiothreitol (DTT) assay ROS, OH, for Anaheim, whereas little observed Beach. These findings highlight interplay various PM redox-active chemical components complex relationship between DTT activity.

Язык: Английский

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Seasonal variation characteristics of hydroxyl radical pollution and its potential formation mechanism during the daytime in Lanzhou

Journal of Environmental Sciences, Год журнала: 2020, Номер 95, С. 58 - 64

Опубликована: Апрель 16, 2020

Язык: Английский

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Proteome-wide effects of naphthalene-derived secondary organic aerosol in BEAS-2B cells are caused by short-lived unsaturated carbonyls

Proceedings of the National Academy of Sciences, Год журнала: 2020, Номер 117(41), С. 25386 - 25395

Опубликована: Сен. 28, 2020

Exposure to air pollution causes adverse health outcomes, but the toxicity mechanisms remain unclear. Here, we investigated dynamic toxicities of naphthalene-derived secondary organic aerosol (NSOA) in a human bronchial epithelial cell line (BEAS-2B) and identified chemical components responsible for toxicities. The composition NSOA was found vary with six simulated atmospheric aging conditions (C1-C6), as characterized by high-resolution mass spectrometry ion mobility spectrometry. Global proteome profiling reveals evolution toxicity: Stronger proteome-wide impacts were detected fresh NSOA, effects declined along aging. While Nrf2-regulated proteins (e.g., NQO1) significantly up-regulated, majority (78 97%) from inflammation other pathways down-regulated exposure Rho GTPases). This pattern is distinct reactive oxygen species (ROS)-mediated pathway, an alternative cysteine reaction pathway revealed decreased abundance MT1X) prone posttranslational thiol modification. further validated observing Nrf2 response reporter cells, after preincubating cysteine. Ethynyl-naphthalene probe employed confirm alkylation cellular thiols on level via in-gel fluorescence imaging. Nontarget analysis several unsaturated carbonyls, including naphthoquinones hydroxylated naphthoquinones, toxic reactivity. Our study provides insights into during identifies short-lived carbonyls predominant at level.

Язык: Английский

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Aqueous-Phase Decomposition of Isoprene Hydroxy Hydroperoxide and Hydroxyl Radical Formation by Fenton-like Reactions with Iron Ions

The Journal of Physical Chemistry A, Год журнала: 2020, Номер 124(25), С. 5230 - 5236

Опубликована: Июнь 1, 2020

Isoprene hydroxy hydroperoxides (ISOPOOH) formed by the photooxidation of isoprene under low-NO conditions play an important role in formation and evolution secondary organic aerosols, yet multiphase processes ISOPOOH are poorly understood. By applying electron paramagnetic resonance spectroscopy, we observe that undergoes aqueous-phase decomposition upon interacting with Fe(II) ions to form OH radicals at room temperature. To reproduce measured dependence on Fe concentrations kinetic modeling, postulate react via Fenton-like reactions a rate constant 7.3 × 10–18 cm3 s–1. At low concentrations, oxalate forms monocomplexes ions, which can promote ISOPOOH. However, high scavenges radicals, thereby lowering aqueous concentrations. These findings provide new insight for atmospheric fate reactive oxygen species generation phase.

Язык: Английский

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Iron-Facilitated Organic Radical Formation from Secondary Organic Aerosols in Surrogate Lung Fluid

Environmental Science & Technology, Год журнала: 2021, Номер 56(11), С. 7234 - 7243

Опубликована: Окт. 1, 2021

Respiratory deposition of secondary organic aerosols (SOA) and iron may lead to the generation reactive oxygen species free radicals in lung fluid cause oxidative stress, but their underlying mechanism formation kinetics are not well understood. Here we demonstrate substantial surrogate (SLF) by mixtures Fe2+ SOA generated from photooxidation isoprene, α-terpineol, toluene. The molar yields measured be 0.03–0.5% SLF, which 5–10 times higher than water. We observe that enhances radical dramatically a factor 20–80, can attributed Fe2+-facilitated decomposition peroxides, consistency with positive correlation between peroxide contents yields. Ascorbate mediates redox cycling ions sustain decomposition, as supported kinetic modeling reproducing time- concentration-dependence additional experiments observing ascorbate Fe3+. •OH superoxide found scavenged antioxidants efficiently. These findings have implications on role damage lipid peroxidation.

Язык: Английский

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Inter-comparison of oxidative potential metrics for airborne particles identifies differences between acellular chemical assays

Atmospheric Pollution Research, Год журнала: 2022, Номер 13(12), С. 101596 - 101596

Опубликована: Ноя. 22, 2022

Oxidative potential (OP) has been identified as an important factor underlying the health effects of airborne particulate matter (PM). OP denotes ability PM to deplete antioxidants and form reactive oxygen species (ROS) in lung. can be quantified using a variety chemical assays analytical techniques. Despite widespread use various metrics, there is no consensus or comprehensive inter-laboratory assessment on how these compare. In this work for first time, we compared 11 indicators from acellular standard reference material urban PM. The included ascorbic acid, glutathione, glutathione disulfide, cysteine, cystine, dithiothreitol, H2O2, •OH, O2•-, empirical theoretical redox simulated lung lining fluid (SLF). showed first-order kinetics at low concentration (25 μg mL−1), whereas were non-linear higher concentrations. demonstrated mainly linear dose-response relationships concentrations 25–100 mL−1, following similar trends with water-soluble transition metals, but they not always proportional concentrations, substantial differences their sensitivities results indicate importance reduced reaction time reliable quantification due non-linearity assay responses high This shows that choice molecular probes measurement techniques must carefully considered when planning studies ambient air should importantly include association metrics outcomes.

Язык: Английский

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Seasonal variation of water-soluble brown carbon in Qingdao, China: Impacts from marine and terrestrial emissions

Environmental Research, Год журнала: 2022, Номер 212, С. 113144 - 113144

Опубликована: Март 24, 2022

Язык: Английский

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