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Annual Review of Physical Chemistry

Volume 75, 2024

Molecular Insights into Chemical Reactions at Aqueous Aerosol Interfaces

Abstract

Atmospheric aerosols facilitate reactions between ambient gases and dissolved species. Here, we review our efforts to interrogate the uptake of these gases and the mechanisms of their reactions both theoretically and experimentally. We highlight the fascinating behavior of NO in solutions ranging from pure water to complex mixtures, chosen because its aerosol-mediated reactions significantly impact global ozone, hydroxyl, and methane concentrations. As a hydrophobic, weakly soluble, and highly reactive species, NO is a sensitive probe of the chemical and physical properties of aerosol interfaces. We employ contemporary theory to disentangle the fate of NO as it approaches pure and salty water, starting with adsorption and ending with hydrolysis to HNO, chlorination to ClNO, or evaporation. Flow reactor and gas-liquid scattering experiments probe even greater complexity as added ions, organic molecules, and surfactants alter the interfacial composition and reaction rates. Together, we reveal a new perspective on multiphase chemistry in the atmosphere.

Keyword(s): aerosol-mediated reactions, air-water interfaces, gas uptake, many-body molecular dynamics, multiphase chemistry, reaction-diffusion systems
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/content/journals/10.1146/annurev-physchem-083122-121620
2024-06-28
2025-04-28
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/content/journals/10.1146/annurev-physchem-083122-121620
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Molecular Insights into Chemical Reactions at Aqueous Aerosol Interfaces
Annual Review of Physical Chemistry 75, 111 (2024); https://doi.org/10.1146/annurev-physchem-083122-121620
/content/journals/10.1146/annurev-physchem-083122-121620
/content/journals/10.1146/annurev-physchem-083122-121620
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