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

被引:76
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
相关论文
共 91 条
[1]   Plasma-catalytic dry reforming of methane in an atmospheric pressure AC gliding arc discharge [J].
Abd Allah, Zaenab ;
Whitehead, J. Christopher .
CATALYSIS TODAY, 2015, 256 :76-79
[2]   Comparison of dry reforming of methane in low temperature hybrid plasma-catalytic corona with thermal catalytic reactor over Ni/γ-Al2O3 [J].
Aziznia, Amin ;
Bozorgzadeh, Hamid Reza ;
Seyed-Matin, Naser ;
Baghalha, Morteza ;
Mohamadalizadeh, Ali .
JOURNAL OF NATURAL GAS CHEMISTRY, 2012, 21 (04) :466-475
[3]   Modeling of CO2 Splitting in a Microwave Plasma: How to Improve the Conversion and Energy Efficiency [J].
Berthelot, Antonin ;
Bogaerts, Annemie .
JOURNAL OF PHYSICAL CHEMISTRY C, 2017, 121 (15) :8236-8251
[4]   Modeling of plasma-based CO2 conversion: lumping of the vibrational levels [J].
Berthelot, Antonin ;
Bogaerts, Annemie .
PLASMA SOURCES SCIENCE & TECHNOLOGY, 2016, 25 (04)
[5]   Plasma assisted dry methane reforming using gliding arc gas discharge: Effect of feed gases proportion [J].
Bo, Zheng ;
Yan, Jianhua ;
Li, Xiaodong ;
Chi, Yong ;
Cen, Kefa .
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY, 2008, 33 (20) :5545-5553
[6]   Hybrid Monte Carlo - fluid modeling network for an argon/hydrogen direct current glow discharge [J].
Bogaerts, A ;
Gijbels, R .
SPECTROCHIMICA ACTA PART B-ATOMIC SPECTROSCOPY, 2002, 57 (06) :1071-1099
[7]   Modeling plasma-based CO2 conversion: crucial role of the dissociation cross section [J].
Bogaerts, Annemie ;
Wang, Weizong ;
Berthelot, Antonin ;
Guerra, Vasco .
PLASMA SOURCES SCIENCE & TECHNOLOGY, 2016, 25 (05)
[8]   Plasma-driven dissociation of CO2 for fuel synthesis [J].
Bongers, Waldo ;
Bouwmeester, Henny ;
Wolf, Bram ;
Peeters, Floran ;
Welzel, Stefan ;
van den Bekerom, Dirk ;
den Harder, Niek ;
Goede, Adelbert ;
Graswinckel, Martijn ;
Groen, Pieter Willem ;
Kopecki, Jochen ;
Leins, Martina ;
van Rooij, Gerard ;
Schulz, Andreas ;
Walker, Matthias ;
van de Sanden, Richard .
PLASMA PROCESSES AND POLYMERS, 2017, 14 (06)
[9]  
Cho W., 2004, P 7 INT C CARB DIOX, P205
[10]   Hydrogen-rich gas production from biogas reforming using plasmatron [J].
Chun, Young N. ;
Song, Hyoung W. ;
Kim, Seong C. ;
Lim, Mun S. .
ENERGY & FUELS, 2008, 22 (01) :123-127