The theoretical study on the mechanisms and pathways of the atmospheric CF3O2 + X (X = F, Cl) reactions

被引:8
作者
Li, Hongwei [1 ]
Tang, Yizhen [1 ]
Wang, Rongshun [2 ]
机构
[1] Qingdao Technol Univ, Sch Environm & Municipal Engn, Qingdao 266033, Shandong, Peoples R China
[2] NE Normal Univ, Fac Chem, Inst Funct Mat Chem, Changchun 130024, Jilin, Peoples R China
基金
中国国家自然科学基金;
关键词
CF3O2; Atmospheric reaction; Halogen; Photolysis; ABSOLUTE RATE CONSTANTS; GAS-PHASE REACTIONS; GAUSSIAN-BASIS SETS; AB-INITIO; CHLORINE ATOMS; RADICALS; NO; KINETICS; HO2; OH;
D O I
10.1016/j.comptc.2013.03.006
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
The pathways of CF3O2 reactions with atomic fluorine and chlorine are studied using quantum chemistry methods. The major products in the CF3O2 + Cl reaction are CF3OOCl, formed via association of initial reactants, and CF3O + ClO, formed via the fission of CF3OOCl on the singlet PES. For the CF3O2 + F reaction the major product is CF3OOF. TDDFT (Time-Dependent DFT) calculations indicate that CF3OOCl will readily undergo photolysis, CF3OOF will also undergo photolysis in the stratosphere. (C) 2013 Elsevier B.V. All rights reserved.
引用
收藏
页码:102 / 108
页数:7
相关论文
共 33 条
[1]   A discharge-flow study of the kinetics of the reactions of IO with CH3O2 and CF3O2 [J].
Bale, CSE ;
Canosa-Mas, CE ;
Shallcross, DE ;
Wayne, RP .
PHYSICAL CHEMISTRY CHEMICAL PHYSICS, 2005, 7 (10) :2164-2172
[2]   Master equation analysis of pressure-dependent atmospheric reactions [J].
Barker, JR ;
Golden, DM .
CHEMICAL REVIEWS, 2003, 103 (12) :4577-4591
[3]   DENSITY-FUNCTIONAL THERMOCHEMISTRY .3. THE ROLE OF EXACT EXCHANGE [J].
BECKE, AD .
JOURNAL OF CHEMICAL PHYSICS, 1993, 98 (07) :5648-5652
[4]   CHEMICAL IONIZATION MASS-SPECTROMETRIC STUDIES OF THE GAS-PHASE REACTIONS CF3O2+NO, CF3O+NO, AND CF3O+RH [J].
BEVILACQUA, TJ ;
HANSON, DR ;
HOWARD, CJ .
JOURNAL OF PHYSICAL CHEMISTRY, 1993, 97 (15) :3750-3757
[5]   FLASH-PHOTOLYSIS TIME-RESOLVED MASS-SPECTROMETRIC INVESTIGATIONS OF THE REACTIONS OF CF3O2 AND CF3O RADICALS WITH NO [J].
BHATNAGAR, A ;
CARR, RW .
CHEMICAL PHYSICS LETTERS, 1994, 231 (4-6) :454-459
[6]   Kinetics of the reaction of CF3O2 radicals with O(P-3) atoms [J].
Biggs, P ;
CanosaMas, CE ;
Shallcross, DE ;
Vipond, A ;
Wayne, RP .
JOURNAL OF THE CHEMICAL SOCIETY-FARADAY TRANSACTIONS, 1997, 93 (15) :2477-2480
[7]   Kinetics of the reactions of CF3O2 with OH, HO2 and H [J].
Biggs, P ;
CanosaMas, CE ;
Shallcross, DE ;
Vipond, A ;
Wayne, RP .
JOURNAL OF THE CHEMICAL SOCIETY-FARADAY TRANSACTIONS, 1997, 93 (16) :2701-2705
[8]   Flow tube/LIF measurements of the rate constants for the reactions with NO of CF3O and CF3O2 radicals [J].
Bourbon, C ;
Brioukov, M ;
Hanoune, B ;
Sawerysyn, JP ;
Devolder, P .
CHEMICAL PHYSICS LETTERS, 1996, 254 (3-4) :203-212
[9]   Kinetics of the reactions of CF3O2 radicals with Cl and I atoms [J].
Canosa-Mas, CE ;
Vipond, A ;
Wayne, RP .
PHYSICAL CHEMISTRY CHEMICAL PHYSICS, 1999, 1 (05) :761-766
[10]   Gaussian-4 theory [J].
Curtiss, Larry A. ;
Redfern, Paul C. ;
Raghavachari, Krishnan .
JOURNAL OF CHEMICAL PHYSICS, 2007, 126 (08)