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1.
ChemSusChem ; 10(20): 4025-4036, 2017 10 23.
Article in English | MEDLINE | ID: mdl-28834403

ABSTRACT

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 10 kJ L-1 (or 2.5 eV per molecule) and an energy efficiency of 66 %. CO and H2 are the major products, with the formation of smaller fractions of C2 Hx (x=2, 4, or 6) compounds and H2 O. 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.


Subject(s)
Methane/chemistry , Plasma Gases/chemistry , Carbon Dioxide/chemistry , Kinetics , Thermodynamics
2.
ChemSusChem ; 10(12): 2642-2652, 2017 06 22.
Article in English | MEDLINE | ID: mdl-28481058

ABSTRACT

Low-temperature plasmas are gaining a lot of interest for environmental and energy applications. A large research field in these applications is the conversion of CO2 into chemicals and fuels. Since CO2 is a very stable molecule, a key performance indicator for the research on plasma-based CO2 conversion is the energy efficiency. Until now, the energy efficiency in atmospheric plasma reactors is quite low, and therefore we employ here a novel type of plasma reactor, the gliding arc plasmatron (GAP). This paper provides a detailed experimental and computational study of the CO2 conversion, as well as the energy cost and efficiency in a GAP. A comparison with thermal conversion, other plasma types and other novel CO2 conversion technologies is made to find out whether this novel plasma reactor can provide a significant contribution to the much-needed efficient conversion of CO2 . From these comparisons it becomes evident that our results are less than a factor of two away from being cost competitive and already outperform several other new technologies. Furthermore, we indicate how the performance of the GAP can still be improved by further exploiting its non-equilibrium character. Hence, it is clear that the GAP is very promising for CO2 conversion.


Subject(s)
Carbon Dioxide/chemistry , Plasma Gases/chemistry , Catalysis , Environment
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