A theoretical study on gas-phase reaction of methylketene with OH: mechanism, kinetics, and insights

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作   者：

Zhang, Yunju;  Liu, Yongguo;  Du, Huaming;  Zhao, Meilian;  Sun, Yuxi;  Li, Huirong;  Wang, Zhiguo; 

作者机构：

Beijing Technol & Business Univ BTBU;  Chengdu Univ Tradit Chinese Med;  Mianyang Normal Univ; 

关键词：

ATOMIC-HYDROGEN;  Rate constants;  TEMPERATURE-DEPENDENCE;  AB-INITIO;  CH2CO;  Methylketene;  ABSOLUTE RATE CONSTANTS;  KETENE;  DENSITY FUNCTIONALS;  ELEMENTS;  Atmospheric lifetime;  Reaction mechanism;  OH;  BASIS-SETS;  RADICALS; 

期刊名称：

Structural Chemistry

i s s n：

1040-0400

年卷期：

2022 年 33 卷 1 期

页   码：

49-56

页   码：

摘   要：

The oxidation mechanism of CH3CHCO initiated by OH is systematically studied using quantum theoretical methods. According to thermodynamic research, the dominant channel is the addition of CH3CHCO with OH generating C-IM1 (CH3CHOHCO) and C-IM2 (CH3CHCOOH), and then dissociate to the dominant products P1 (CH3CHO + CO) from C-IM1 with the lowest barrier. The rate constants for CH3CHCO + OH -> C-IM1 -> P1/CH3CHCO + OH -> C-IM2 channels are computed through RRKM theory at 200-2000 K. The obtained overall rate constant at 298 K (7.60 x 10(-11) cm(3) molecule(-1) s(-1)) is well consistent with the reported experimental value. The atmospheric lifetime of CH3CHCO is estimated to be around 1.83 h.