Dataset Information

Measurements of Hydroxyl Radical Concentrations during Indoor Cooking Events: Evidence of an Unmeasured Photolytic Source of Radicals.

ABSTRACT: The hydroxyl radical (OH) is the dominant oxidant in the outdoor environment, controlling the lifetimes of volatile organic compounds (VOCs) and contributing to the growth of secondary organic aerosols. Despite its importance outdoors, there have been relatively few measurements of the OH radical in indoor environments. During the House Observations of Microbial and Environmental Chemistry (HOMEChem) campaign, elevated concentrations of OH were observed near a window during cooking events, in addition to elevated mixing ratios of nitrous acid (HONO), VOCs, and nitrogen oxides (NO_X). Particularly high concentrations were measured during the preparation of a traditional American Thanksgiving dinner, which required the use of a gas stove and oven almost continually for 6 h. A zero-dimensional chemical model underpredicted the measured OH concentrations even during periods when direct sunlight illuminated the area near the window, which increases the rate of OH production by photolysis of HONO. Interferences with measurements of nitrogen dioxide (NO₂) and ozone (O₃) suggest that unmeasured photolytic VOCs were emitted during cooking events. The addition of a VOC that photolyzes to produce peroxy radicals (RO₂), similar to pyruvic acid, into the model results in better agreement with the OH measurements. These results highlight our incomplete understanding of the nature of oxidation in indoor environments.

SUBMITTER: Reidy E

PROVIDER: S-EPMC9850917 | biostudies-literature | 2023 Jan

REPOSITORIES: biostudies-literature

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Measurements of Hydroxyl Radical Concentrations during Indoor Cooking Events: Evidence of an Unmeasured Photolytic Source of Radicals.

Reidy Emily E Bottorff Brandon P BP Rosales Colleen Marciel F CMF Cardoso-Saldaña Felipe J FJ Arata Caleb C Zhou Shan S Wang Chen C Abeleira Andrew A Hildebrandt Ruiz Lea L Goldstein Allen H AH Novoselac Atila A Kahan Tara F TF Abbatt Jonathan P D JPD Vance Marina E ME Farmer Delphine K DK Stevens Philip S PS

Environmental science & technology 20230105 2

The hydroxyl radical (OH) is the dominant oxidant in the outdoor environment, controlling the lifetimes of volatile organic compounds (VOCs) and contributing to the growth of secondary organic aerosols. Despite its importance outdoors, there have been relatively few measurements of the OH radical in indoor environments. During the House Observations of Microbial and Environmental Chemistry (HOMEChem) campaign, elevated concentrations of OH were observed near a window during cooking events, in ad ...[more]

PMID: 36603843

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Project description:The atmospheric oxidation of organics occurs primarily via reaction cycles involving gas phase radical species, catalysed by nitric oxide (NO), which result in the production of secondary pollutants such as ozone. For these oxidation cycles to occur, they must be initialized by a primary radical, i.e., a radical formed from non-radical precursors. Once formed, these primary radicals can result in the oxidation of organic compounds to produce peroxy radicals that, providing sufficient NO is present, can re-generate "secondary" radicals which can go on to oxidize further organics. Thus, one primary radical can result in the catalytic oxidation of multiple organics. Although the photolysis of ozone in the presence of water vapor to form two hydroxyl (OH) radicals is accepted as the dominant tropospheric primary radical source, multiple other primary radical sources exist and can dominate in certain environments. The chemical reactivity of different radicals to organic and inorganic compounds can be very different, however, and how these differences in radical chemistry impact atmospheric organic oxidation under different atmospheric conditions has not been previously demonstrated. In this work, we use a series of model simulations to investigate the impact of the chemical reactivity of the primary radical on the effectiveness in initializing organic oxidation and thus the production of the secondary pollutant ozone. We compare the chemistries of the OH and atomic chlorine (Cl) radicals and their effectiveness at initializing organic oxidation under different nitrogen oxide and organic concentrations. The OH radical is the dominant tropospheric radical, with both primary and secondary sources. In contrast, Cl has primary sources that show significant spatial heterogeneity throughout the troposphere but is not typically regenerated in catalytic cycles. Both primary OH and Cl can initiate organic oxidation, but this work shows that the relative effectiveness with which they oxidize organics and produce ozone depends on their balance of propagation vs termination reactions which is in turn determined by the chemical environment in which they are produced. In particular, our work shows that in high NOx radical-limited environments, like those found in many urban areas, Cl will be more efficient at oxidizing organics than OH.

Dataset Information

Measurements of Hydroxyl Radical Concentrations during Indoor Cooking Events: Evidence of an Unmeasured Photolytic Source of Radicals.

Publications

Measurements of Hydroxyl Radical Concentrations during Indoor Cooking Events: Evidence of an Unmeasured Photolytic Source of Radicals.

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