CO2–CH4 conversion and syngas formation at atmospheric pressure using a multi-electrode dielectric barrier discharge

Ozkan, A; Dufour, Thierry; Arnoult, G.; Keyzer, Philippe De; Bogaerts, Annemie; Reniers, François

doi:10.1016/j.jcou.2015.01.002

Cited by 103 publications

(56 citation statements)

References 53 publications

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“…Because of its advantages over conventional reforming technologies, a lot of research has already been devoted to the plasma‐based conversion of greenhouse gases into value‐added products. Most of the research has been based on pure CO 2 splitting or dry reforming of methane . Pure H 2 O plasmas for the production of hydrogen have also been extensively studied .…”

Section: Introductionmentioning

confidence: 99%

The Quest for Value‐Added Products from Carbon Dioxide and Water in a Dielectric Barrier Discharge: A Chemical Kinetics Study

et al. 2016

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Recycling of carbon dioxide by its conversion into value-added products has gained significant interest owing to the role it can play for use in an anthropogenic carbon cycle. The combined conversion with H O could even mimic the natural photosynthesis process. An interesting gas conversion technique currently being considered in the field of CO conversion is plasma technology. To investigate whether it is also promising for this combined conversion, we performed a series of experiments and developed a chemical kinetics plasma chemistry model for a deeper understanding of the process. The main products formed were the syngas components CO and H , as well as O and H O , whereas methanol formation was only observed in the parts-per-billion to parts-per-million range. The syngas ratio, on the other hand, could easily be controlled by varying both the water content and/or energy input. On the basis of the model, which was validated with experimental results, a chemical kinetics analysis was performed, which allowed the construction and investigation of the different pathways leading to the observed experimental results and which helped to clarify these results. This approach allowed us to evaluate this technology on the basis of its underlying chemistry and to propose solutions on how to further improve the formation of value-added products by using plasma technology.

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Section: Introductionmentioning

confidence: 99%

The Quest for Value‐Added Products from Carbon Dioxide and Water in a Dielectric Barrier Discharge: A Chemical Kinetics Study

et al. 2016

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“…Moreover, a DBD reactor has a simple design that can easily be up-scaled for industrial applications, as already demonstrated for the ozone synthesis [30][31][32]. We have already demonstrated that our flowing DBD setup presents a good compromise between a reasonable energy efficiency and a high CO2 conversion for low specific energy input (SEI) [33].…”

Section: Note: This Document Is a Pre-print Version You May Use It Amentioning

confidence: 75%

The influence of power and frequency on the filamentary behavior of a flowing DBD—application to the splitting of CO₂

Özkan

Dufour

Silva

et al. 2016

Plasma Sources Sci. Technol.

115

117

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In this experimental study, a flowing dielectric barrier discharge operating at atmospheric pressure is used for the splitting of CO2 into O2 and CO. The influence of the applied frequency and plasma power on the microdischarge properties is investigated to understand their role on the CO2 conversion. Electrical measurements are carried out to explain the conversion trends and to characterize the microdischarges through their number, their lifetime, their intensity and the induced electrical charge. Their influence on the gas and electrode temperatures is also evidenced through optical emission spectroscopy and infrared imaging. It is shown that, in our configuration, the conversion depends mostly on the charge delivered in the plasma and not on the effective plasma voltage when the applied power is modified. Similarly, at constant total current, a better conversion is observed at low frequencies, where a less filamentary discharge regime with a higher effective plasma voltage than that at a higher frequency is obtained.

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“…6 illustrates the various experimental data for energy efficiency vs. total conversion, obtained from literature, [25][26][27][28]32,33 in comparison with our simulation results, for all conditions investigated. 6 illustrates the various experimental data for energy efficiency vs. total conversion, obtained from literature, [25][26][27][28]32,33 in comparison with our simulation results, for all conditions investigated.…”

Section: Model Predictions In a Wider Parameter Rangementioning

confidence: 94%

Plasma-based dry reforming: improving the conversion and energy efficiency in a dielectric barrier discharge

et al. 2015

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Dry reforming of methane has gained significant interest over the years. A novel reforming technique with great potential is plasma technology. One of its drawbacks, however, is energy consumption. Therefore, we performed an extensive computational study, supported by experiments, aiming to identify the influence of the operating parameters (gas mixture, power, residence time and "frequency") of a dielectric barrier discharge plasma on the conversion and energy efficiency, and to investigate which of these parameters lead to the most promising results and whether these are eventually sufficient for industrial implementation. The best results, in terms of both energy efficiency and conversion, are obtained at a specific energy input (SEI) of 100 J cm À3 , a 10-90 CH 4 -CO 2 ratio, 10 Hz, a residence time of 1 ms, resulting in a total conversion of 84% and an energy efficiency of 8.5%. In general, increasing the CO 2 content in the gas mixture leads to a higher conversion and energy efficiency. The SEI couples the effect of the power and residence time, and increasing the SEI always results in a higher conversion, but somewhat lower energy efficiencies. The effect of the frequency is more complicated: we observed that the product of frequency (f) and residence time (s), being a measure for the total number of microdischarge filaments which the gas molecules experience when passing through the reactor, was critical.For most cases, a higher number of filaments yields higher values for conversion and energy efficiency. To benchmark our model predictions, we also give an overview of measured conversions and energy efficiencies reported in the literature, to indicate the potential for improvement compared to the state-ofthe art. Finally, we identify the limitations as well as the benefits and future possibilities of plasma technology. † Electronic supplementary information (ESI) available: The ESI contains (a) an overview of the detailed experimental and computational results, used for the model validation; as a function of the CH 4 -CO 2 ratio, the residence time and the SEI. (b) All graphs and a more extensive description of the inuence regarding gas ratio in the entire range of conditions. See

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CO2–CH4 conversion and syngas formation at atmospheric pressure using a multi-electrode dielectric barrier discharge

Cited by 103 publications

References 53 publications

The Quest for Value‐Added Products from Carbon Dioxide and Water in a Dielectric Barrier Discharge: A Chemical Kinetics Study

The Quest for Value‐Added Products from Carbon Dioxide and Water in a Dielectric Barrier Discharge: A Chemical Kinetics Study

The influence of power and frequency on the filamentary behavior of a flowing DBD—application to the splitting of CO₂

Plasma-based dry reforming: improving the conversion and energy efficiency in a dielectric barrier discharge

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CO2–CH4 conversion and syngas formation at atmospheric pressure using a multi-electrode dielectric barrier discharge

Cited by 103 publications

References 53 publications

The Quest for Value‐Added Products from Carbon Dioxide and Water in a Dielectric Barrier Discharge: A Chemical Kinetics Study

The Quest for Value‐Added Products from Carbon Dioxide and Water in a Dielectric Barrier Discharge: A Chemical Kinetics Study

The influence of power and frequency on the filamentary behavior of a flowing DBD—application to the splitting of CO2

Plasma-based dry reforming: improving the conversion and energy efficiency in a dielectric barrier discharge

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The influence of power and frequency on the filamentary behavior of a flowing DBD—application to the splitting of CO₂