Abstract
The O(3P)-initiated conversion mechanism and dynamics of CH3CHCO were researched in atmosphere by executing density functional theory (DFT) computations. Optimizations of all the species and single-point energy computations were implemented at the B3LYP/6–311++G(d,p) and CCSD(T)/cc-pVTZ level, respectively. The explicit oxidation mechanism was introduced and discussed. The results state clearly that the O(3P) association was more energetically beneficial than the abstraction of H. The rate coefficients over the probable temperature range of 200–3000 K were forecasted by implementing Rice-Ramsperger-Kassel-Marcus (RRKM) theory. Specifically, the total rate coefficient of O(3P) association reactions is 1.19 × 10−11 cm3 molecule−1 s−1 at 298 K, which is consistent with the experimental results (1.16 × 10−11 cm3 molecule−1 s−1). The rate coefficients for the O(3P) with CH2CO, CH3CHCO, and (CH3)2CCO suggest that rate coefficient of ketene derivatives increase with the increase of methylation degree.
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This work was supported by the Natural Science Foundations of China (No. 21707062) and Scientific Research Starting Foundation of Mianyang Normal University (No. QD2016A007) and supported by the Open Project Program of Beijing Key Laboratory of Flavor Chemistry, Beijing Technology and Business University (BTBU), Beijing 100048, China.
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Yongguo Liu, Huaming Du, Meilian Zhao, Yuxi Sun, Huirong Li Zhiguo Wang: Calculation, data curation, formal analysis, and investigation. Yunju Zhang: calculation and writing-review and editing
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Zhang, Y., Liu, Y., Zhao, M. et al. Theoretical investigations on mechanisms and kinetics of methylketene with O(3P) reaction in the atmosphere. J Mol Model 27, 228 (2021). https://doi.org/10.1007/s00894-021-04850-w
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DOI: https://doi.org/10.1007/s00894-021-04850-w