The number fraction of iron-containing particles affects OH, HO<sub>2</sub> and H<sub>2</sub>O<sub>2</sub> budgets in the atmospheric aqueous phase DOI Creative Commons

Amina Khaled,

Minghui Zhang, Barbara Ervens

и другие.

Atmospheric chemistry and physics, Год журнала: 2022, Номер 22(3), С. 1989 - 2009

Опубликована: Фев. 11, 2022

Abstract. Reactive oxygen species (ROS), such as OH, HO2 and H2O2, affect the oxidation capacity of atmosphere cause adverse health effects particulate matter. The role transition metal ions (TMIs) in impacting ROS concentrations conversions atmospheric aqueous phase has been recognized for a long time. Model studies usually assume that total TMI mass measured bulk aerosol or cloud water samples is distributed equally across all particles droplets. This assumption contrary to single-particle measurements have shown only small number fraction contain iron other TMIs (FN,Fe<100 %), which implies also not droplets TMIs. In current study, we apply box model with an explicit multiphase chemical mechanism simulate formation cycling simulations are performed range 1 % ≤ FN,Fe 100 constant pH values 3, 4.5 6 concentration (10 50 ng per cubic meter air). results compared two sets FN,Fe<100 (FeN<100) (FeBulk). We find largest differences between OH / O2- at = 6. Under these conditions, subsaturated because its high effective Henry's law fast loss reactions radical anion. As main reduction process Fe(III) reaction O2-, show subsaturation leads Fe(II) Fe(total) ratios lower by factor 2 approaches. trend largely independent concentration, both source sink rates scale concentration. compare model-derived reactive uptake parameters γOH γHO2 full FN,Fe. While affected distribution, calculated from 0.0004 0.03 %, respectively. Implications findings discussed application lab-derived models present on aerosols. conclude distribution (FN,Fe) should be taken into account estimate potential matter might overestimated sampling Our study suggests iron-containing may more important than determining budgets water.

Язык: Английский

Wildfire particulate matter as a source of environmentally persistent free radicals and reactive oxygen species DOI Creative Commons
Ting Fang, Brian C. H. Hwang, Sukriti Kapur

и другие.

Environmental Science Atmospheres, Год журнала: 2023, Номер 3(3), С. 581 - 594

Опубликована: Янв. 1, 2023

Wildfire particulate matter contains high amounts of environmentally persistent free radicals and generates reactive oxygen species with implications for air quality public health.

Язык: Английский

Процитировано

23
Iron-Facilitated Organic Radical Formation from Secondary Organic Aerosols in Surrogate Lung Fluid DOI
Jinlai Wei, Ting Fang, Pascale S. J. Lakey

и другие.

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

Процитировано

39
Aqueous OH Radical Production by Brake Wear Particles DOI Creative Commons
Ting Fang, Sukriti Kapur, Kasey C. Edwards

и другие.

Environmental Science & Technology Letters, Год журнала: 2024, Номер 11(4), С. 315 - 322

Опубликована: Март 25, 2024

Particulate matter (PM) emitted from road traffic causes adverse health effects upon inhalation and respiratory deposition. Non-exhaust emissions will eventually become the dominant source of PM transition to electric vehicles; however, non-tailpipe is currently unregulated as its impacts are still unclear. In this study, we generated brake wear particles (BWPs) with non-asbestos organic, ceramic, semimetallic pads using custom dynamometers measured aqueous-phase formation reactive oxygen species (ROS). We found that BWPs do not contain environmentally persistent free radicals (EPFRs), all types generate exclusively ·OH in water. by ceramic brakes during heavier braking lead higher yields compared gentle conditions, suggesting potential ultrafine BWPs. Chemical characterization reveals organic elemental carbon correlated positively while exhibiting negative correlations abundant metals including Fe Mn. suggest thermal decomposition hydroperoxides derived phenolic resin. oxidative quantified dithiothreitol (DTT) assay exhibited a positive correlation yield. These results provide critical insights into toxicity

Язык: Английский

Процитировано

6
Superoxide Release by Macrophages through NADPH Oxidase Activation Dominating Chemistry by Isoprene Secondary Organic Aerosols and Quinones to Cause Oxidative Damage on Membranes DOI Creative Commons
Ting Fang,

Yu-Kai Huang,

Jinlai Wei

и другие.

Environmental Science & Technology, Год журнала: 2022, Номер 56(23), С. 17029 - 17038

Опубликована: Ноя. 17, 2022

Oxidative stress mediated by reactive oxygen species (ROS) is a key process for adverse aerosol health effects. Secondary organic aerosols (SOA) account major fraction of fine particulate matter, and their inhalation deposition into the respiratory tract causes formation ROS chemical cellular processes, but relative contributions are hardly quantified link to oxidative remains uncertain. Here, we superoxide generation 9,10-phenanthrenequinone (PQN) isoprene SOA using chemiluminescence assay combined with electron paramagnetic resonance spectroscopy as well kinetic modeling. We also applied imaging techniques study mechanism release damage on cell membranes. show that PQN activate NADPH oxidase in macrophages massive amounts superoxide, overwhelming aqueous reactions epithelial lining fluid. The activation dose 2 orders magnitude lower than SOA, suggesting quinones more toxic. While higher exposures trigger antioxidant response elements, released induce membrane through lipid peroxidation. Such mechanistic quantitative understandings provide basis further elucidation effects matter.

Язык: Английский

Процитировано

23
Effects of Nitrogen Oxides on the Production of Reactive Oxygen Species and Environmentally Persistent Free Radicals from α-Pinene and Naphthalene Secondary Organic Aerosols DOI Creative Commons
Kasey C. Edwards, Alexandra L. Klodt, Tommaso Galeazzo

и другие.

The Journal of Physical Chemistry A, Год журнала: 2022, Номер 126(40), С. 7361 - 7372

Опубликована: Окт. 4, 2022

Reactive oxygen species (ROS) and environmentally persistent free radicals (EPFR) play an important role in chemical transformation of atmospheric aerosols adverse aerosol health effects. This study investigated the effects nitrogen oxides (NOx) during photooxidation α-pinene naphthalene on EPFR content ROS formation from secondary organic (SOA). Electron paramagnetic resonance (EPR) spectroscopy was applied to quantify formation. While no were detected SOA, we found that SOA contained about 0.7 pmol μg-1 EPFR, NOx has little influence concentrations oxidative potential. α-Pinene generated under low conditions form OH superoxide aqueous phase, which lowered substantially by 50-80% for high conditions. High-resolution mass spectrometry analysis showed substantial nitroaromatics nitrates a environment. The modeling results using GECKO-A model simulates explicit gas-phase chemistry radical 2D-VBS treats autoxidation predicted reduced hydroperoxides enhanced due reactions peroxy with instead their HO2. Consistently, presence resulted decrease peroxide contents potential SOA.

Язык: Английский

Процитировано

22
Isomer-Resolved Reactivity of Organic Peroxides in Monoterpene-Derived Secondary Organic Aerosol DOI
Min Yao, Ziyue Li, Chenxi Li

и другие.

Environmental Science & Technology, Год журнала: 2022, Номер 56(8), С. 4882 - 4893

Опубликована: Март 31, 2022

Organic peroxides play a vital role in the formation, evolution, and health impacts of atmospheric aerosols, yet their molecular composition fate particle phase remain poorly understood. Here, we identified, using iodometry-assisted liquid chromatography mass spectrometry, large suite isomer-resolved peroxide monomers (C8-10H12-18O5-8) dimers (C15-20H22-34O5-14) secondary organic aerosol formed from ozonolysis most abundant monoterpene (α-pinene). Combining isothermal evaporation experiments multilayer kinetic modeling, bulk were found to undergo rapid particle-phase chemical transformation with an average lifetime several hours under humid conditions, while individual decompose on timescales half hour few days. Meanwhile, majority isomeric exhibit distinct behaviors, highlighting importance characterization reactivity. Furthermore, reactivity increases water content faster low relative humidity (RH) range than high RH range. Such non-uniform effects imply more important as plasticizer reactant influencing The its striking dependence should be considered modeling chemistry effects.

Язык: Английский

Процитировано

21
Photoenhanced Radical Formation in Aqueous Mixtures of Levoglucosan and Benzoquinone: Implications to Photochemical Aging of Biomass-Burning Organic Aerosols DOI Creative Commons
Lena Gerritz, Meredith Schervish, Pascale S. J. Lakey

и другие.

The Journal of Physical Chemistry A, Год журнала: 2023, Номер 127(24), С. 5209 - 5221

Опубликована: Июнь 7, 2023

The photochemical aging of biomass-burning organic aerosols (BBOAs) by exposure to sunlight changes the chemical composition over its atmospheric lifetime, affecting toxicological and climate-relevant properties BBOA particles. This study used electron paramagnetic resonance (EPR) spectroscopy with a spin-trapping agent, 5-tert-butoxycarbonyl-5-methyl-1-pyrroline-N-oxide (BMPO), high-resolution mass spectrometry, kinetic modeling photosensitized formation reactive oxygen species (ROS) free radicals in mixtures benzoquinone levoglucosan, known tracer molecules. EPR analysis irradiated solutions showed dominant hydroxyl (•OH), which are products reaction triplet-state water, also yielding semiquinone radicals. In addition, hydrogen (H•) were observed, not detected previous studies. They most likely generated decomposition irradiation levoglucosan led substantial carbon- oxygen-centered radicals, became prominent higher fraction levoglucosan. High-resolution spectrometry permitted direct observation BMPO-radical adducts demonstrated •OH, derived from oxidation Mass superoxide radical (BMPO-OOH) that did appear spectra. Kinetic processes successfully reproduced time evolution observed BMPO •OH H• EPR. model was then applied describe would occur absence BMPO, predicting generation HO2• due dissolved oxygen. These results imply photoirradiation containing photosensitizers induces ROS secondary chemistry drive atmosphere.

Язык: Английский

Процитировано

12
Dynamic Oxidative Potential of Organic Aerosol from Heated Cooking Oil DOI

Shunyao Wang,

Manpreet Takhar, Yue Zhao

и другие.

ACS Earth and Space Chemistry, Год журнала: 2021, Номер 5(5), С. 1150 - 1162

Опубликована: Апрель 19, 2021

Cooking emissions contribute significantly to organic aerosol in urban areas, but the evolution of physicochemical properties and health impacts upon atmospheric aging remain poorly understood. In this study, detailed chemical composition oxidative potential (OP) primary (POA) secondary (SOA) from heated cooking oils (canola, olive, peanut) were characterized. Results acellular measurements indicate an enhanced OP photochemically aged SOA compared that POA, which is accompanied by increasing abundance reactive oxygen species (ROS) measured using electron paramagnetic resonance (EPR) spectroscopy. canola oil, total ROS production (by a factor 26) coincides with increased particle-phase peroxide content (from 15 26%) across six different photooxidation conditions (up 2 days equivalent). Positive correlations found among abundance, content, average carbon oxidation state oil along aging. Photooxidation representative volatile compounds shows unsaturated aldehydes are dominant contributors peroxides during aging, degree unsaturation aldehyde precursor linked ROS/peroxide SOA. The abundant OH radicals suggest major radical source SOA, likely initiated homolytic cleavage oxygen–oxygen single bond. Our study bridges shedding light on their dynamic toxicity atmosphere.

Язык: Английский

Процитировано

24
Chemical Fate of Oils on Indoor Surfaces: Ozonolysis and Peroxidation DOI
Zilin Zhou, Leigh R. Crilley, Jenna C. Ditto

и другие.

Environmental Science & Technology, Год журнала: 2023, Номер 57(41), С. 15546 - 15557

Опубликована: Авг. 30, 2023

Unsaturated triglycerides found in food and skin oils are reactive ambient air. However, the chemical fate of such compounds has not been well characterized genuine indoor environments. Here, we monitored aging oil coatings on glass surfaces over a range environmental conditions, using mass spectrometry, nuclear magnetic resonance (NMR), electron paramagnetic (EPR) techniques. Upon room air exposure (up to 17 ppb ozone), characteristic ozonolysis products, secondary ozonides, were observed near cooking area commercial kitchen, along with condensed-phase aldehydes. In an office setting, is also dominant degradation pathway for films exposed enclosed spaces as drawers, depleted flow makes lipid autoxidation more favorable after induction period few days. Forming hydroperoxides major primary this radical-mediated peroxidation behavior accelerated by direct sunlight, but initiation step dark settings still unclear. These results accord radical measurements, indicating that photooxidation facilitates formation surfaces. Overall, many intermediate end products oxygen species (ROS) may induce oxidative stress human bodies. Given these can be widely both household surfaces, their toxicological properties worth further attention.

Язык: Английский

Процитировано

11
Influence of ambient and endogenous H2O2 on reactive oxygen species concentrations and OH radical production in the respiratory tract DOI Creative Commons
Eleni Dovrou, Steven Lelieveld, Ashmi Mishra

и другие.

Environmental Science Atmospheres, Год журнала: 2023, Номер 3(7), С. 1066 - 1074

Опубликована: Янв. 1, 2023

A multiphase kinetic model analysis quantifies effects of air pollutants on reactive oxygen species production and oxidative stress in the respiratory tract.

Язык: Английский

Процитировано

10