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The gas-phase reaction of organic acids with SO3 has been recognized as essential in promoting aerosol particle formation. However, this reaction at the air-water interface is poorly understood. Herein, we performed systematic Born-Oppenheimer molecular dynamics (BOMD) simulations to study the reaction of various organic acids with SO3 on the surface of a water droplet. The results show that at the air-water interface, the organic acid-SO3 reaction follows a distinctly different mechanism than that in the gas phase. At the interface, the reaction occurs on the picosecond scale, within which the ion pairs of sulphuric-carboxylic anhydride and hydronium form. This distinct reaction mechanism at the aqueous surface has important atmospheric implications, e.g., promoting water condensation, uptaking atmospheric condesation species, and incorporating "SO42-" into organic species in aerosol particles. Therefore, the reaction acts as another path towards aerosol formation under humid conditions.
This article was published in the following journal.
Name: Angewandte Chemie (International ed. in English)
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Compounds derived from organic or inorganic acids in which at least one hydroxyl group is replaced by an –O-alkyl or other organic group. They can be represented by the structure formula RCOOR’ and are usually formed by the reaction between an acid and an alcohol with elimination of water.
Aminobenzenesulfonic acids. Organic acids that are used in the manufacture of dyes and organic chemicals and as reagents.
Organic compounds that are acyclic and contain three acid groups. A member of this class is citric acid which is the first product formed by reaction of pyruvate and oxaloacetate. (From Lehninger, Principles of Biochemistry, 1982, p443)
Organic, monobasic acids derived from hydrocarbons by the equivalent of oxidation of a methyl group to an alcohol, aldehyde, and then acid. Fatty acids are saturated and unsaturated (FATTY ACIDS, UNSATURATED). (Grant & Hackh's Chemical Dictionary, 5th ed)
Organic compounds containing the carboxy group (-COOH). This group of compounds includes amino acids and fatty acids. Carboxylic acids can be saturated, unsaturated, or aromatic.