Dry Reforming of Methane in a Gliding Arc Plasmatron: Towards a Better Understanding of the Plasma Chemistry

被引:73
|
作者
Cleiren, Emelie [1 ]
Heijkers, Stijn [1 ]
Ramakers, Marleen [1 ]
Bogaerts, Annemie [1 ]
机构
[1] Univ Antwerp, Dept Chem, Res Grp PLASMANT, Univ Pl 1, B-2610 Antwerp, Belgium
关键词
CO2; conversion; dry reforming; hydrogen; kinetics; plasma chemistry; DIELECTRIC-BARRIER DISCHARGE; CO2-CONTAINING NATURAL-GAS; CARBON-DIOXIDE; HIGHER HYDROCARBONS; MICROWAVE PLASMA; ENERGY EFFICIENCY; SPARK-DISCHARGE; NONTHERMAL PLASMA; DIRECT CONVERSION; CORONA PLASMA;
D O I
10.1002/cssc.201701274
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
Dry reforming of methane (DRM) in a gliding arc plasmatron is studied for different CH4 fractions in the mixture. The CO2 and CH4 conversions reach their highest values of approximately 18 and 10%, respectively, at 25% CH4 in the gas mixture, corresponding to an overall energy cost of 10kJL(-1) (or 2.5eV per molecule) and an energy efficiency of 66%. CO and H-2 are the major products, with the formation of smaller fractions of C2Hx (x=2, 4, or 6) compounds and H2O. A chemical kinetics model is used to investigate the underlying chemical processes. The calculated CO2 and CH4 conversion and the energy efficiency are in good agreement with the experimental data. The model calculations reveal that the reaction of CO2 (mainly at vibrationally excited levels) with H radicals is mainly responsible for the CO2 conversion, especially at higher CH4 fractions in the mixture, which explains why the CO2 conversion increases with increasing CH4 fraction. The main process responsible for CH4 conversion is the reaction with OH radicals. The excellent energy efficiency can be explained by the non-equilibrium character of the plasma, in which the electrons mainly activate the gas molecules, and by the important role of the vibrational kinetics of CO2. The results demonstrate that a gliding arc plasmatron is very promising for DRM.
引用
收藏
页码:4025 / 4036
页数:12
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