Rapid heterogeneous oxidation of organic coatings on submicron aerosols

Lim, Christopher Y.; Browne, E. C.; Sugrue, Rebecca A.; Kroll, J. H.

doi:10.1002/2017gl072585

Cited by 33 publications

(70 citation statements)

References 50 publications

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“…However, SOA rapidly starts to cover the surface of the SPs, and the particle constitution may be described by a core–shell model. Only particulate organic species at or near the particle surface are exposed to OH radicals, whereas the soot core of the particle is shielded against heterogeneous oxidation ( Lim et al. 2017 ).…”

Section: Methodsmentioning

confidence: 99%

Effect of Atmospheric Aging on Soot Particle Toxicity in Lung Cell Models at the Air–Liquid Interface: Differential Toxicological Impacts of Biogenic and Anthropogenic Secondary Organic Aerosols (SOAs)

Offer

Hartner

Bucchianico

et al. 2022

Environ Health Perspect

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Section: Methodsmentioning

confidence: 99%

Effect of Atmospheric Aging on Soot Particle Toxicity in Lung Cell Models at the Air–Liquid Interface: Differential Toxicological Impacts of Biogenic and Anthropogenic Secondary Organic Aerosols (SOAs)

Offer

Hartner

Bucchianico

et al. 2022

Environ Health Perspect

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“…Over the span of atmospheric lifetime, the mass and chemical composition of SOA can be affected by aging processes Lim et al, 2017). The aerosol aging processes that we studied here include oligomerization, heterogeneous oxidation, and metal mixing.…”

Section: Discussionmentioning

confidence: 99%

Relationship between chemical composition and oxidative potential of secondary organic aerosol from polycyclic aromatic hydrocarbons

Wang

Soong

et al. 2018

Atmos. Chem. Phys.

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Abstract. Owing to the complex nature and dynamic behaviors of secondary organic aerosol (SOA), its ability to cause oxidative stress (known as oxidative potential, or OP) and adverse health outcomes remains poorly understood. In this work, we probed the linkages between the chemical composition of SOA and its OP, and investigated impacts from various SOA evolution pathways, including atmospheric oligomerization, heterogeneous oxidation, and mixing with metal. SOA formed from photooxidation of the two most common polycyclic aromatic hydrocarbons (naphthalene and phenanthrene) were studied as model systems. OP was evaluated using the dithiothreitol (DTT) assay. The oligomerrich fraction separated by liquid chromatography dominates DTT activity in both SOA systems (52 ± 10 % for naphthalene SOA (NSOA), and 56 ± 5 % for phenanthrene SOA (PSOA)). Heterogeneous ozonolysis of NSOA was found to enhance its OP, which is consistent with the trend observed in selected individual oxidation products. DTT activities from redox-active organic compounds and metals were found to be not additive. When mixing with highly redox-active metal (Cu), OP of the mixture decreased significantly for 1,2-naphthoquinone (42 ± 7 %), 2,3-dihydroxynaphthalene (35 ± 1 %), NSOA (50 ± 6 %), and PSOA (43 ± 4 %). Evidence from proton nuclear magnetic resonance ( 1 H NMR) spectroscopy illustrates that such OP reduction upon mixing can be ascribed to metal-organic binding interactions. Our results highlight the role of aerosol chemical composition under atmospheric aging processes in determining the OP of SOA, which is needed for more accurate and explicit prediction of the toxicological impacts from particulate matter.

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“…These, together with the ability to rapidly achieve high photochemical ages, are advantageous for field applications. These advantages of OFRs have led a number of atmospheric chemistry research groups (Lambe and Jimenez, 2018) to deploy them in field (Hu et al, 2016;Ortega et al, 2016;Palm et al, 2016Palm et al, , 2017, source Tkacik et al, 2014;Karjalainen et al, 2016;Link et al, 2016) and laboratory studies (Kang et al, 2011;Lambe et al, 2013;Richards-Henderson et al, 2016;Lim et al, 2017).…”

Section: Introductionmentioning

confidence: 99%

Organic peroxy radical chemistry in oxidation flow reactors and environmental chambers and their atmospheric relevance

et al. 2019

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Abstract. Oxidation flow reactors (OFRs) are a promising complement to environmental chambers for investigating atmospheric oxidation processes and secondary aerosol formation. However, questions have been raised about how representative the chemistry within OFRs is of that in the troposphere. We investigate the fates of organic peroxy radicals (RO2), which play a central role in atmospheric organic chemistry, in OFRs and environmental chambers by chemical kinetic modeling and compare to a variety of ambient conditions to help define a range of atmospherically relevant OFR operating conditions. For most types of RO2, their bimolecular fates in OFRs are mainly RO2+HO2 and RO2+NO, similar to chambers and atmospheric studies. For substituted primary RO2 and acyl RO2, RO2+RO2 can make a significant contribution to the fate of RO2 in OFRs, chambers and the atmosphere, but RO2+RO2 in OFRs is in general somewhat less important than in the atmosphere. At high NO, RO2+NO dominates RO2 fate in OFRs, as in the atmosphere. At a high UV lamp setting in OFRs, RO2+OH can be a major RO2 fate and RO2 isomerization can be negligible for common multifunctional RO2, both of which deviate from common atmospheric conditions. In the OFR254 operation mode (for which OH is generated only from the photolysis of added O3), we cannot identify any conditions that can simultaneously avoid significant organic photolysis at 254 nm and lead to RO2 lifetimes long enough (∼ 10 s) to allow atmospherically relevant RO2 isomerization. In the OFR185 mode (for which OH is generated from reactions initiated by 185 nm photons), high relative humidity, low UV intensity and low precursor concentrations are recommended for the atmospherically relevant gas-phase chemistry of both stable species and RO2. These conditions ensure minor or negligible RO2+OH and a relative importance of RO2 isomerization in RO2 fate in OFRs within ∼×2 of that in the atmosphere. Under these conditions, the photochemical age within OFR185 systems can reach a few equivalent days at most, encompassing the typical ages for maximum secondary organic aerosol (SOA) production. A small increase in OFR temperature may allow the relative importance of RO2 isomerization to approach the ambient values. To study the heterogeneous oxidation of SOA formed under atmospherically relevant OFR conditions, a different UV source with higher intensity is needed after the SOA formation stage, which can be done with another reactor in series. Finally, we recommend evaluating the atmospheric relevance of RO2 chemistry by always reporting measured and/or estimated OH, HO2, NO, NO2 and OH reactivity (or at least precursor composition and concentration) in all chamber and flow reactor experiments. An easy-to-use RO2 fate estimator program is included with this paper to facilitate the investigation of this topic in future studies.

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Rapid heterogeneous oxidation of organic coatings on submicron aerosols

Cited by 33 publications

References 50 publications

Effect of Atmospheric Aging on Soot Particle Toxicity in Lung Cell Models at the Air–Liquid Interface: Differential Toxicological Impacts of Biogenic and Anthropogenic Secondary Organic Aerosols (SOAs)

Effect of Atmospheric Aging on Soot Particle Toxicity in Lung Cell Models at the Air–Liquid Interface: Differential Toxicological Impacts of Biogenic and Anthropogenic Secondary Organic Aerosols (SOAs)

Relationship between chemical composition and oxidative potential of secondary organic aerosol from polycyclic aromatic hydrocarbons

Organic peroxy radical chemistry in oxidation flow reactors and environmental chambers and their atmospheric relevance

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