Kinetics for the reaction of Criegee intermediate CH2OO with n-butyraldehyde and its atmospheric implications
|Corresponding Author||Ding，Hongbin; Dong，Wenrui|
The Criegee intermediates (CIs), formed through ozone oxidation of unsaturated hydrocarbons, can undergo reactions with various carbonyl compounds in the atmosphere. In this study, we have investigated the 1,3-cycloaddition reaction of n-butyraldehyde with the simplest Criegee intermediate, CHOO, using the OH laser-induced fluorescence (LIF) method. The experiments were conducted over a temperature and pressure range of 283–318 K and 5–100 Torr, respectively. Our results reveal that the bimolecular rate constant of the reaction is dependent on both temperature and pressure. Specifically, the measured rate constants at 100 Torr are (3.51 ± 0.63), (2.97 ± 0.53), (2.70 ± 0.49), and (2.52 ± 0.45) × 10 cm molecule s at temperatures of 283, 298, 308, and 318 K, respectively, with a total error of 18%. By fitting the pressure-dependent rate constants according to the Lindemann mechanism, we obtained a high-pressure limit rate constant of (3.05 ± 0.55) × 10 cm molecule s at 298 K. The Arrhenius plot of the temperature-dependent rate constants yields an activation energy of (−1.71 ± 0.30) kcal mol and a pre-exponential factor of (1.66 ± 0.24) × 10 cm s (total error). Furthermore, our findings indicate that the title reaction exhibits a more pronounced temperature-dependent effect compared to that of CHOO with water dimer and SO, as well as that of OH with n-butyraldehyde. This observation suggests that the significance of title reaction in the atmosphere increases at lower temperature.
National Natural Science Foundation of China;National Natural Science Foundation of China;Chinese Academy of Sciences[GJJSTD20220001];Liaoning Revitalization Talents Program[XLYC1807248];
|WOS Research Area|
Environmental Sciences & Ecology ; Meteorology & Atmospheric Sciences
Environmental Sciences ; Meteorology & Atmospheric Sciences
|WOS Accession No|
|ESI Research Field|
Cited Times [WOS]:0
|Document Type||Journal Article|
|Department||Department of Chemistry|
1.Key Laboratory of Materials Modification by Laser,Ion,and Electron Beams,Chinese Ministry of Education,School of Physics,Dalian University of Technology,Dalian,116024,China
2.State Key Laboratory of Molecular Reaction Dynamics,Dalian Institute of Chemical Physics,Chinese Academy of Sciences,Dalian,116023,China
3.Key Laboratory of Chemical Lasers,Dalian Institute of Chemical Physics,Chinese Academy of Sciences,Dalian,116023,China
4.University of Chinese Academy of Sciences,Beijing,100049,China
5.Department of Chemical Physics,School of Chemistry and Materials Science,University of Science and Technology of China,Hefei,230026,China
6.Department of Physics,Dalian Maritime University,Dalian,Liaoning,116026,China
7.Department of Chemistry,Southern University of Science and Technology,Shenzhen,518055,China
Liu，Siyue,Chen，Yang,Jiang，Haotian,et al. Kinetics for the reaction of Criegee intermediate CH2OO with n-butyraldehyde and its atmospheric implications[J]. Atmospheric Environment,2023,311.
Liu，Siyue.,Chen，Yang.,Jiang，Haotian.,Shi，Jiayu.,Ding，Hongbin.,...&Dong，Wenrui.(2023).Kinetics for the reaction of Criegee intermediate CH2OO with n-butyraldehyde and its atmospheric implications.Atmospheric Environment,311.
Liu，Siyue,et al."Kinetics for the reaction of Criegee intermediate CH2OO with n-butyraldehyde and its atmospheric implications".Atmospheric Environment 311(2023).
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