Molecular-Scale Mechanism of Sequential Reaction of Oxalic Acid with SO3: Potential Participator in Atmospheric Aerosol Nucleation

Ye Yang, Ling Liu*, Huixian Wang, Xiuhui Zhang*

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

13 Citations (Scopus)

Abstract

Recent research has shown the almost barrierless cycloaddition reaction of the carboxylic acid with one SO3 to form products with group of -OSO3H, which can form stable clusters with the nucleation precursors through hydrogen bonds (Mackenzie et al., Science 2015, 349, 58). Oxalic acid (OA), the simplest and prevalent dicarboxylic acid, was selected as an example to clarify the possibility to react with two SO3 sequentially and the nucleation potential of products. The results indicate that OA can sequentially react with two SO3 through low reaction barriers to form the primary product (oxalic sulfuric anhydride (OSA)) and the secondary product (oxalic disulfuric anhydride (ODSA)). Interactions between atmospheric nucleation precursors and OSA, ODSA, or OA are in the order of ODSA > OSA > OA through evaluating the stability of generated clusters by the topological, thermodynamics, and kinetic analysis, which implies generated products could be nucleation stabilizers with nucleation potential positively correlating with the number of -OSO3H. This reaction mechanism contributes to a comprehensive understanding of the reactivity of dicarboxylic acid in the polluted environment as well as the role of products in organosulfur chemistry and, to some extent, help to explain the missing sources of new particle formation.

Original languageEnglish
Pages (from-to)4200-4208
Number of pages9
JournalJournal of Physical Chemistry A
Volume125
Issue number19
DOIs
Publication statusPublished - 20 May 2021

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