Evidence of Surface-Tension Lowering of Atmospheric Aerosols by Organics from Field Observations in an Urban Atmosphere: Relation to Particle Size and Chemical Composition

Fan, Tianyi; Ren, Jingye; Liu, Chenxi; Li, Z.; Liu, Jieyao; Sun, Yele; Wang, Yuying; Jin, Xiaoai; Zhang, Fang

doi:10.1021/acs.est.4c03141

Environ. Sci. Technol.

2024

DOI: 10.1021/acs.est.4c03141

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Evidence of Surface-Tension Lowering of Atmospheric Aerosols by Organics from Field Observations in an Urban Atmosphere: Relation to Particle Size and Chemical Composition

Tianyi Fan,

Jingye Ren,

Chenxi Liu

et al.

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2024

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Cited by 3 publications

References 94 publications

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Surface Nitrate Enrichment and Enhanced HONO Production from Ionic Surfactant Aggregation at the Aqueous-Air Interface

Li,

Ma,

et al. 2024

Environ. Sci. Technol.

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Significant discrepancies persist between field observations and model simulations regarding the strength of marine-derived HONO sources, underscoring the urgency to resolve unidentified HONO sources. In this study, sodium dodecyl sulfate (SDS) was chosen as a proxy for marine surfactants to investigate its impact on aqueous nitrate photolysis for the first time. Remarkable increases in HONO and NO 2 production rates by factors of 3.3 and 5.6, respectively, along with a 1.9-fold rise in NO 2 − concentration, were observed at a very low SDS concentration of 0.01 mM, strongly illustrating the promoting effect on nitrate photolysis. Furthermore, at an SDS concentration of 2 mM, intriguingly aligned with the critical micelle concentration, there was an additional 41.7% increase in HONO production rates. Vertically resolved Raman measurements indicated that SDS anions at the aqueous-air interface attracted NO 3 − closer to the aqueous surfaces, increasing the amount of incompletely solvated surface nitrate. Importantly, the anionic surfactant exhibited a greater promoting effect on HONO production compared to other typical nitrate photochemistry systems with the addition of a marine dissolved organic matter proxy, halogen, photosensitizer, or OH scavenger. These findings offer new insights into marine-derived HONO sources and should be considered in model simulations concerning the budgets of NO x , OH, and O 3 .

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Surface Nitrate Enrichment and Enhanced HONO Production from Ionic Surfactant Aggregation at the Aqueous-Air Interface

Li,

Ma,

et al. 2024

Environ. Sci. Technol.

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Model-Measurement Comparisons for Surfactant-Containing Aerosol Droplets

Bain,

Prisle,

Bzdek

2024

ACS Earth Space Chem.

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Surfactants are important components of atmospheric aerosols, potentially impacting their hygroscopic growth and eventual activation into cloud droplets. By adsorbing at the air−water interface, surfactants lower the surface tension of aqueous systems. However, in microscopic aerosol droplets, the bulk surfactant concentration can become depleted because of the droplets' high surfacearea-to-volume ratio, reducing the bulk surfactant concentration at equilibrium and increasing droplet surface tension. Partitioning models have been developed to account for the concentration-and size-dependencies of surface tension, but these models have rarely been assessed against experimentally measured droplet surface tensions. Here, we directly compare surface tension predictions made using a simple kinetic partitioning model and a thermodynamic monolayer partitioning model against experimentally measured picoliter droplet surface tensions for 12 surfactant− cosolute systems. Surface tension predictions were also made across 8 orders of magnitude in droplet radius. The largest differences between model predictions were associated with the predicted onset of bulk depletion. The quality of the isotherm or parametrization fit to the macroscopic data most strongly influenced a model's ability to accurately predict droplet surface tension. These results highlight the importance of validating partitioning models against droplet surface tension measurements in size ranges where bulk depletion is expected to occur and motivate collection of high-quality macroscopic surface tension data sets that serve as model inputs. The results also validate both models' abilities to predict aerosol surface tension across size and composition, which will facilitate their eventual incorporation into cloud parcel models to explore the impact of surface tension assumptions on cloud droplet number concentration.

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Hygroscopic behavior and aerosol chemistry of atmospheric particles containing organic acids and inorganic salts

Tan,

Zhang,

Xia

et al. 2024

npj Clim Atmos Sci

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Aerosol hygroscopic behavior plays a central role in determining climate effects and environmental influence of atmospheric particulates. Water-soluble organic acids (WSOAs) constitute a significant fraction of organic aerosols. These organic acids have a complex impact on aerosol hygroscopicity due to their physical and chemical interactions with atmospheric inorganic salts. The mixing of WSOAs with inorganic salts exerts a multiple influence on the hygroscopic growth and phase behaviors of aerosol particles, largely depending on the composition ratio, acid properties, particle size and interactions between particle components. The WSOAs play a critical role in determining water uptake characteristics of aerosol particles, especially in the low and moderate RH ranges. The previous studies reveal the occurrence of aerosol chemistry related to chloride/nitrate/ammonium depletions in aerosol droplets containing WSOAs and inorganic salts. The potential influence of WSOAs on the atmospheric recycling of HCl/HNO3/NH3 due to the chloride/nitrate/ammonium depletion may contribute to the atmospheric budget of reactive gases. A fundamental understanding for the hygroscopic behavior and aerosol chemistry of inorganic–WSOA systems is essential for the accurate parameterization of aerosol behaviors in atmospheric models. However, there is still lack of a comprehensive understanding of the hygroscopicity and related aerosol chemistry of internally mixed inorganic–WSOA systems. The present review comprehensively summarizes the impacts of WSOAs on hygroscopicity and phase changes of atmospherically relevant inorganic salts in aerosol particles especially under subsaturated conditions, and overviews the recent advances on aerosol chemistry related to the hygroscopic process for the internally mixed inorganic–WSOA aerosols.

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Evidence of Surface-Tension Lowering of Atmospheric Aerosols by Organics from Field Observations in an Urban Atmosphere: Relation to Particle Size and Chemical Composition

Cited by 3 publications

References 94 publications

Surface Nitrate Enrichment and Enhanced HONO Production from Ionic Surfactant Aggregation at the Aqueous-Air Interface

Surface Nitrate Enrichment and Enhanced HONO Production from Ionic Surfactant Aggregation at the Aqueous-Air Interface

Model-Measurement Comparisons for Surfactant-Containing Aerosol Droplets

Hygroscopic behavior and aerosol chemistry of atmospheric particles containing organic acids and inorganic salts

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