The simplest Criegee intermediate CH2OO reaction with dimethylamine and trimethylamine: kinetics and atmospheric implications

Chen，Yang1,2,3; Zhong，Licheng3,4; Liu，Siyue3,5; Jiang，Haotian3,6; Shi，Jiayu3,7; Jin，Yuqi2,3; Yang，Xueming3,8; Dong，Wenrui3,9

2023-08-09

10.1039/d3cp02948d

Physical Chemistry Chemical Physics   影响因子和分区

1463-9076

1463-9084

We have used the OH laser-induced fluorescence (LIF) method to measure the kinetics of the simplest Criegee intermediate (CHOO) reacting with two abundant amines in the atmosphere: dimethylamine ((CH)NH) and trimethylamine ((CH)N). Our experiments were conducted under pseudo-first-order approximation conditions. The rate coefficients we report are (2.15 ± 0.28) × 10 cm molecule s for (CH)NH at 298 K and 10 Torr, and (1.56 ± 0.23) × 10 cm molecule s for (CH)N at 298 K and 25 Torr with Ar as the bath gas. Both reactions exhibit a negative temperature dependence. The activation energy and pre-exponential factors derived from the Arrhenius equation were (−2.03 ± 0.26) kcal mol and (6.89 ± 0.90) × 10 cm molecule s for (CH)NH, and (−1.60 ± 0.24) kcal mol and (1.06 ± 0.16) × 10 cm molecule s for (CH)N. We propose that the electronegativity of the atom in the co-reactant attached to the C atom of CHOO, in addition to the dissociation energy of the fragile covalent bonds with H atoms (H-X bond), plays an important role in the 1,2-insertion reactions. Under certain circumstances, the title reactions can contribute to the sink of amines and Criegee intermediates and to the formation of secondary organic aerosol (SOA).

SCI ; EI

英语

其他

National Natural Science Foundation of China (NSFC)[22288201] ; Chinese Academy of Sciences[GJJSTD20220001] ; Innovation Program for Quantum Science and Technology[2021ZD0303305]

Chemistry ; Physics

Chemistry, Physical ; Physics, Atomic, Molecular & Chemical

WOS:001051988200001

ROYAL SOC CHEMISTRY

20233614674965

Activation energy ; Atoms ; Chemical bonds ; Electronegativity ; Molecules ; Reaction intermediates ; Reaction kinetics ; Temperature distribution

Thermodynamics:641.1 ; Physical Chemistry:801.4 ; Electrochemistry:801.4.1 ; Chemical Reactions:802.2 ; Chemical Products Generally:804 ; Organic Compounds:804.1 ; Atomic and Molecular Physics:931.3

CHEMISTRY

2-s2.0-85169184072

Scopus

1.Key Laboratory of Chemical Lasers,Dalian Institute of Chemical Physics,Chinese Academy of Sciences,Dalian,116023,China
2.University of Chinese Academy of Sciences,Beijing,100049,China
3.State Key Laboratory of Molecular Reaction Dynamics,Dalian Institute of Chemical Physics,Chinese Academy of Sciences,Dalian,116023,China
4.College of Chemical Engineering,Shenyang University of Chemical Technology,Shenyang,110142,China
5.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
6.Department of Chemical Physics,School of Chemistry and Materials Science,University of Science and Technology of China,Hefei,230026,China
7.Department of Physics,Dalian Maritime University,Dalian,Liaoning,116026,China
8.Department of Chemistry,Southern University of Science and Technology,Shenzhen,518055,China
9.Hefei National Laboratory,Hefei,230088,China

Chen，Yang,Zhong，Licheng,Liu，Siyue,et al. The simplest Criegee intermediate CH2OO reaction with dimethylamine and trimethylamine: kinetics and atmospheric implications[J]. Physical Chemistry Chemical Physics,2023,25(34):23187-23196.

Chen，Yang.,Zhong，Licheng.,Liu，Siyue.,Jiang，Haotian.,Shi，Jiayu.,...&Dong，Wenrui.(2023).The simplest Criegee intermediate CH2OO reaction with dimethylamine and trimethylamine: kinetics and atmospheric implications.Physical Chemistry Chemical Physics,25(34),23187-23196.

Chen，Yang,et al."The simplest Criegee intermediate CH2OO reaction with dimethylamine and trimethylamine: kinetics and atmospheric implications".Physical Chemistry Chemical Physics 25.34(2023):23187-23196.