Conversion of CHF3 to CH2=CF2 via reaction with CH4 in the presence of CBrF3: An experimental and kinetic modelling study

被引:21
作者
Han, Wenfeng [1 ]
Kennedy, Eric M. [1 ]
Mackie, John C. [1 ]
Dlugogorski, Bogdan Z. [1 ]
机构
[1] Univ Newcastle, PRCfE Sch Engn, Proc Safety & Environm Protect Res Grp, Callaghan, NSW 2308, Australia
基金
澳大利亚研究理事会;
关键词
Trifluoromethane; Greenhouse gas; Methane; Halon; Vinylidene fluoride; Hydrofluorocarbon; GAS-PHASE REACTION; REAL-TIME; BROMINATION; PYROLYSIS; METHANE; TRIFLUOROMETHANE; DISSOCIATION; FLUOROFORM; DECOMPOSITION; SELECTIVITY;
D O I
10.1016/j.jhazmat.2010.04.011
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
Gas-phase reaction of CHF3 (HFC 23) with CH4 in the presence of CBrF3 (halon 1301) to produce CH2=CF2 (VDF) is presented. Experiments were carried out in a plug-flow reactor at temperatures between 873 and 1173 K. Under these conditions, CH2=CF2 was a dominant product observed, with CH2F2, C2H2, CH2CHF, C2F4, C2H6 and CHFCF2 also detected. In the presence of less than 6000 ppm of CBrF3, the rate of formation of CH2=CF2 is significantly enhanced, and a much lower rate of formation of the major by-product, C2F4 is observed. Further increasing the proportion of CBrF3 in the feed resulted in an even higher rate of formation of CH2=CF2. Experimental results are fitted very well by a model derived from the NIST and GRI-Mech 3.0 mechanisms, modified to include additional published kinetic data. (C) 2010 Elsevier B.V. All rights reserved.
引用
收藏
页码:181 / 187
页数:7
相关论文
共 44 条
[1]   Fluoroelastomers:: synthesis, properties and applications [J].
Améduri, B ;
Boutevin, B ;
Kostov, G .
PROGRESS IN POLYMER SCIENCE, 2001, 26 (01) :105-187
[2]   BROMINATION OF FLUOROALKANES .4. KINETICS OF THERMAL BROMINATION OF FLUOROFORM AND PENTAFLUOROETHANE [J].
AMPHLETT, JC ;
WHITTLE, E .
TRANSACTIONS OF THE FARADAY SOCIETY, 1968, 64 (548P) :2130-&
[3]  
[Anonymous], CATAL TODAY
[4]  
[Anonymous], AM0001 INC HFC 23 WA
[5]   Emission profiles from the foam and refrigeration sectors comparison with atmospheric concentrations. Part 2: results and discussion [J].
Ashford, P ;
Clodic, D ;
McCulloch, A ;
Kuijpers, L .
INTERNATIONAL JOURNAL OF REFRIGERATION-REVUE INTERNATIONALE DU FROID, 2004, 27 (07) :701-716
[6]   Influence of CF3I, CF3Br, and CF3H on the high-temperature combustion of methane [J].
Babushok, V ;
Noto, T ;
Burgess, DRF ;
Hamins, A ;
Tsang, W .
COMBUSTION AND FLAME, 1996, 107 (04) :351-367
[7]  
BURAVTSEV NN, 1994, DOKL AKAD NAUK+, V339, P616
[8]   Effects of C-H stretch excitation on the H+CH4 reaction -: art. no. 134301 [J].
Camden, JP ;
Bechtel, HA ;
Brown, DJA ;
Zare, RN .
JOURNAL OF CHEMICAL PHYSICS, 2005, 123 (13)
[9]   CORRELATION OF ACTIVATION ENERGIES + BOND ENERGIES IN CF3 REACTIONS [J].
CARMICHAEL, H ;
JOHNSTON, HS .
JOURNAL OF CHEMICAL PHYSICS, 1964, 41 (07) :1975-&
[10]   VAPOUR-PHASE BROMINATION OF FLUOROFORM AND METHANE [J].
CORBETT, P ;
TARR, AM ;
WHITTLE, E .
TRANSACTIONS OF THE FARADAY SOCIETY, 1963, 59 (487) :1609-&