ArticleThe journal of physical chemistry. A2026
Reaction Kinetics of Methyl Vinyl Ketone Oxide with Carboxylic Acids: Experimental and Theoretical Insights into Atmospheric Conditions.
Article in The journal of physical chemistry. A, 2026. The graph could read no effect estimate from its abstract, so it casts no vote on the map. Not yet cited in PubMed.
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Abstract
Criegee intermediates (CIs) formed via alkene ozonolysis play an important role in tropospheric oxidation chemistry. Methyl vinyl ketone oxide (MVKO), an isoprene-derived CI, is expected to have a significant impact in regions with high biogenic emissions; however, quantitative kinetic data for reactions with organic acids remain limited. Here, the reaction kinetics of MVKO with acetic acid (CH3COOH) and propionic acid (CH3CH2COOH) were investigated using time-resolved cavity ring-down spectroscopy (TR-CRDS) at 298 K under low pressure conditions. The measured bimolecular rate coefficients are (2.7 ± 0.1) × 10-10 and (3.6 ± 0.1) × 10-10 cm3 molecule-1 s-1 for CH3COOH and CH3CH2COOH, respectively, indicating near-collision-limited reactivity. Complementary quantum chemical calculations combined with variational transition state theory identify barrierless reaction pathways for MVKO reactions with carboxylic acids, driven by the formation of strong hydrogen-bonding interactions. The calculated high-pressure-limit rate coefficients are in good agreement with the experimental values, with small deviations attributable to falloff effects. Incorporating the derived kinetics into a chemical transport model indicates that reactions with organic acids provide an efficient sink for MVKO in isoprene-rich regions, leading to a maximum reduction of approximately 3% in the carboxylic acid concentration. These results provide robust kinetic constraints for MVKO-acid reactions and improve the representation of isoprene-derived CI chemistry in atmospheric models.
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