Plasma reforming of methane in a tunable ferroelectric packed-bed dielectric barrier discharge reactor

Montoro-Damas, Antonio M.; Brey, J.J.; Rodríguez, Miguel Á.; González‐Elipe, Agustín R.; Cotrino, José

doi:10.1016/j.jpowsour.2015.07.038

Cited by 31 publications

(27 citation statements)

References 32 publications

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“…Their shape is quite similar to that recorded when operating the reactor with a mixture N 2 + H 2 , thus indicating that the two reaction mixtures behave similarly. Unlike the oval shape of the Lissajous curve obtained when operating the reactor in the conventional AC sinusoidal mode [12] used for the wet reforming reaction [3], the square shape of the Lissajous curves in Figure 5 is consistent with the fact that we are operating the reactor with a squared AC voltage in a packed bed reactor. Furthermore, the non-centered Lissajous figure is in agreement with the asymmetric squared signal.…”

Section: Methodssupporting

confidence: 68%

“…), there is still limited knowledge about the influence of other working parameters, such as the residence time of the reactants, internal structure of the reactors, and therefore the distribution of gases within the discharge, and so on. In recent works on the synthesis of ammonia [9,11] and on the reforming of hydrocarbons [3,12], we have demonstrated how the reaction performance is affected by these parameters. In particular, using deuterated water for the wet reforming reaction of methane, we were able to prove that not only direct reactions transforming the reactants (methane and water) intro products (hydrogen and carbon Monoxide) take place in the plasma, but also a panoply of intermediate processes that, consuming energy, do not lead to the formation of new product molecules [3].…”

Section: Introductionmentioning

confidence: 93%

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Isotope Labelling for Reaction Mechanism Analysis in DBD Plasma Processes

et al. 2019

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Dielectric barrier discharge (DBD) plasmas and plasma catalysis are becoming an alternative procedure to activate various gas phase reactions. A low-temperature and normal operating pressure are the main advantages of these processes, but a limited energy efficiency and little selectivity control hinder their practical implementation. In this work, we propose the use of isotope labelling to retrieve information about the intermediate reactions that may intervene during the DBD processes contributing to a decrease in their energy efficiency. The results are shown for the wet reforming reaction of methane, using D2O instead of H2O as reactant, and for the ammonia synthesis, using NH3/D2/N2 mixtures. In the two cases, it was found that a significant amount of outlet gas molecules, either reactants or products, have deuterium in their structure (e.g., HD for hydrogen, CDxHy for methane, or NDxHy for ammonia). From the analysis of the evolution of the labelled molecules as a function of power, useful information has been obtained about the exchange events of H by D atoms (or vice versa) between the plasma intermediate species. An evaluation of the number of these events revealed a significant progression with the plasma power, a tendency that is recognized to be detrimental for the energy efficiency of reactant to product transformation. The labelling technique is proposed as a useful approach for the analysis of plasma reaction mechanisms.

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Section: Methodssupporting

confidence: 68%

Section: Introductionmentioning

confidence: 93%

Isotope Labelling for Reaction Mechanism Analysis in DBD Plasma Processes

et al. 2019

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“…However, although a large variety of reactor set-ups and working conditions have been proposed to maximize the efficiency of these processes [19][20][21][22][23], most studies have addressed the kinetics of the removal process and paid little attention to the analysis of the plasma, the electrical operation parameters or the effect of the reactor configuration. Common working conditions in these works are a low concentration of pollutants in air, of the order of hundreds or, maximum, thousands ppms, and the pursuit of the full oxidation of VOCs to CO 2 Advanced arrangements of DBD reactors for gas reaction processes such as the reforming of hydrocarbons, CO 2 conversion or the synthesis of ammonia incorporate a ferroelectric moderator between the metallic electrodes [24][25][26][27][28]. This design is advantageous with respect to classical configurations incorporating dielectric materials because the operating voltages can be smaller [29,30] and high plasma currents can be maintained for relatively large separation gaps between electrodes [31,32].…”

Section: Introductionmentioning

confidence: 99%

Improving the pollutant removal efficiency of packed-bed plasma reactors incorporating ferroelectric components

Gómez‐Ramírez

Montoro-Damas

Rodríguez

et al. 2017

Chemical Engineering Journal

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“…The phenomenon can be attributed to various different factors: formation of streamers between particles (reduction of discharge gap), formation of surface streamers on particles, and formation of streamers inside the particle pores. 68 We attribute this both to the zeolite being highly porous as well as having more uneven shape, providing more points of low distance discharge pathways between the particles, and effects such as electric field edge effect.…”

Section: Effect Of the In-plasma Materials On The Discharge Propertiesmentioning

confidence: 99%

“…67 Another thing to be considered is also the effect of frequency on the discharge properties coupled with a packing material, which we did not study in this work but can be seen elsewhere. 68…”

Section: Effect Of the In-plasma Materials On The Discharge Propertiesmentioning

confidence: 99%

Plasma‐activated methane partial oxidation reaction to oxygenate platform chemicals over Fe, Mo, Pd and zeolite catalysts

et al. 2019

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Summary Natural gas from stranded sources is being predominantly flared, and there is a growing demand for new technologies for its utilisation, where electrification, flexibility, and modularity play an important role. Plasma‐activated methane partial oxidation reaction was studied in a designed dielectric barrier discharge ionisation reactor unit, producing value‐added platform chemicals, namely, methanol, formaldehyde, intermediate formic acid, acetic acid, and paraformaldehyde at ambient temperature and atmospheric pressure. The effects of various process parameters, such as voltage, total convertible gas flow rate, and reagent ratio relationship, were considered. In addition, coupling of the following catalytic materials with plasma was examined: alumina (Al2O3), chabazite, ferrierite, microporous beta zeolite, silica (SiO2) glass beads, ZSM‐5 (MFI), Fe on H‐ZSM‐5 and Al2O3, Mo on H‐ZSM‐5, TiO2 and SiO2, and Pd on Al2O3. In the liquid product, 21.5% CH3OH, 20.4% CH2O, 0.3% HCOOH, and 2.4% CH3COOH were measured when using pure plasma, and a maximum aggregate yield of the organic oxygenate compounds of 5.21 mol.% was achieved. The usage of shaped silicate surface increased the selectivity towards synthesised oxygen‐containing structures, while the application of alumino‐silicate mixture constituents reduced it. It was determined that elementary covalently bonded carbon was formed inside pores when pure zeolites were used. Fe‐ and Pd‐based heterogeneous catalysts favoured the complete exothermic combustion of CH4 feedstock reactant species, and the liquid product consisted only of water in the Pd‐ case. The utilisation of Mo/H‐ZSM‐5 resulted in a 46% increased yield of formalin. A mechanism for the role of Mo was proposed, where Mo oxidises methanol to formaldehyde and the metal is reoxidised in plasma.

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Plasma reforming of methane in a tunable ferroelectric packed-bed dielectric barrier discharge reactor

Cited by 31 publications

References 32 publications

Isotope Labelling for Reaction Mechanism Analysis in DBD Plasma Processes

Isotope Labelling for Reaction Mechanism Analysis in DBD Plasma Processes

Improving the pollutant removal efficiency of packed-bed plasma reactors incorporating ferroelectric components

Plasma‐activated methane partial oxidation reaction to oxygenate platform chemicals over Fe, Mo, Pd and zeolite catalysts

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