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Kinetics of the Simplest Criegee Intermediate CH2OO Reacting with CF3CF=CF2
Yang Chen1,2,3, Xiao-hu Zhou3,4, Yi-qiang Liu3,5, Yu-qi Jin1, Wen-rui Dong*1, Xue-ming Yang*3,6
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.State Key Laboratory of Fine Chemicals and Key Laboratory of Industrial Ecology and Environmental Engineering, School of Environmental Science & Technology, Dalian University of Technology, Dalian 116024, China;5.Key Laboratory of Materials Modi cation by Laser, Ion and Electron Beams (Ministry of Education), School of Physics, Dalian University of Technology, Dalian 116024, China;6.Department of Chemistry, Southern University of Science and Technology, Shenzhen 518055, China
Abstract:
CF3CF=CF2 is a potential source of atmospheric trifluoroacetic acid (CF3C(O)OH). The kinetics of the reaction of the simplest Criegee intermediate (CH2OO) with CF3CF=CF2 was studied by using the OH laser-induced fluorescence method. At 10 torr, the rate co-efficients were measured to be (1.45±0.14)×10?13, (1.18±0.11)×10?13, (1.11±0.08)×10?13, and (1.04±0.08)×10?13·cm3·molecule?1·s?1 at 283, 298, 308 and 318 K, respectively. The activation energy of (-1.66±0.21) kcal/mol was derived from the Arrhenius equation. No obvious pressure dependence was observed.
Key words:  Criegee Intermediate, Reaction kinetics, Rate coefficient
FundProject:
附件
克里奇中间体CH2OO与CF3CF=CF2反应的动力学研究
陈 旸1,2,3, 周小虎3,4, 刘义强3,5, 金玉奇1, 董文锐*3, 杨学明*3,6
1.中国科学院大连化学物理研究所化学激光重点实验室,大连 116023;2.中国科学院大学,北京 100049;3.中国科学院大连化学物理研究所分子反应动力学国家重点实验室,大连 116023;4.大连理工大学环境学院,精细化工国家重点实验室和工业生态与环境工程重点实验室,大连 116024;5.大连理工大学物理学院,三束材料改性重点实验室,大连 116024;6.南方科技大学化学系,深圳 518055
摘要:
本文使用OH激光诱导荧光方法研究了结构最简单的克里奇中间体CH2OO和CF3CF=CF2的反应动力学. 在压强为10 Torr条件下,测量了温度在283,298,308和318 K的反应速率常数,分别为(1.45±0.14)×10-13,(1.18±0.11)×10-13,(1.11±0.08)×10-13和(1.04±0.08)×10-13 cm3·molecule-1·s-1. 根据阿伦尼乌斯方程,获得该反应的活化能为(-1.66±0.21) kcal/mol. 在6.3∽70 torr压力范围内,未观察到该反应的速率常数存在压力相关.
关键词:  克里奇中间体,反应动力学,速率常数
DOI:10.1063/1674-0068/cjcp2002025
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