High energy efficiency in syngas and hydrocarbon production from dissociation of CH<sub>4</sub>–CO<sub>2</sub>mixture in a non-equilibrium pulsed plasma

Ghorbanzadeh, A. M.; Norouzi, Samira; Mohammadi, Toraj

doi:10.1088/0022-3727/38/20/006

Cited by 37 publications

(15 citation statements)

References 28 publications

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“…[63] Atmospheric pressure glow discharges also seem to be promising for DRM, with maximum conversionso f3 5-85% and energyc osts of 1-60 eV per molecule. [74][75][76][77][78][79] Clearly,t he GAP is among the most promising types of plasmas forD RM in terms of energy cost or energy efficiency.I n Ref. [72] Finally,n anosecond-pulsedp lasmasp rovidedc onversions between 1a nd 60 %f or energy costs between 3a nd 100 eV per molecule.…”

Section: Resultsmentioning

confidence: 99%

“…[72] Finally,n anosecond-pulsedp lasmasp rovidedc onversions between 1a nd 60 %f or energy costs between 3a nd 100 eV per molecule. [74][75][76][77][78][79] Clearly,t he GAP is among the most promising types of plasmas forD RM in terms of energy cost or energy efficiency.I n Ref. [2],amaximum energy cost of 4.27 eV per molecule correspondingt oaminimum energy efficiency of 60 %( assuming that syngasw as the only product formed) was proposed as the target for plasma-based DRM to become industrially competitive with classical and other novel conversion technologies.…”

Section: Measured Conversion Energy Efficiencya Nd Energycostmentioning

confidence: 99%

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

et al. 2017

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Dry reforming of methane (DRM) in a gliding arc plasmatron is studied for different CH fractions in the mixture. The CO and CH conversions reach their highest values of approximately 18 and 10 %, respectively, at 25 % CH in the gas mixture, corresponding to an overall energy cost of 10 kJ L (or 2.5 eV per molecule) and an energy efficiency of 66 %. CO and H are the major products, with the formation of smaller fractions of C H (x=2, 4, or 6) compounds and H O. A chemical kinetics model is used to investigate the underlying chemical processes. The calculated CO and CH conversion and the energy efficiency are in good agreement with the experimental data. The model calculations reveal that the reaction of CO (mainly at vibrationally excited levels) with H radicals is mainly responsible for the CO conversion, especially at higher CH fractions in the mixture, which explains why the CO conversion increases with increasing CH fraction. The main process responsible for CH 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 CO . The results demonstrate that a gliding arc plasmatron is very promising for DRM.

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Section: Resultsmentioning

confidence: 99%

Section: Measured Conversion Energy Efficiencya Nd Energycostmentioning

confidence: 99%

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

et al. 2017

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“…They can be combusted with oxygen for the production of electricity or heat, but they can also be used as a carbon source in the manufacture of commodity chemicals [249]. This can be achieved by means of reforming methane to synthesis gas (CO/H 2 ) and subsequently using syngas in industrial processes such as methanol synthesis, ammonia synthesis, hydrogenations or Fischer-Tropsch (FT) reactions [250,251]. There are three oxidative routes to generate syngas from methane: partial oxidation (Equation (2)), steam reforming (Equation 3) and dry reforming (Equation 4).…”

Section: Dry Reforming Of Hydrocarbonsmentioning

confidence: 99%

Ceria-Based Catalysts Studied by Near Ambient Pressure X-ray Photoelectron Spectroscopy: A Review

et al. 2020

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The development of better catalysts is a passionate topic at the forefront of modern science, where operando techniques are necessary to identify the nature of the active sites. The surface of a solid catalyst is dynamic and dependent on the reaction environment and, therefore, the catalytic active sites may only be formed under specific reaction conditions and may not be stable either in air or under high vacuum conditions. The identification of the active sites and the understanding of their behaviour are essential information towards a rational catalyst design. One of the most powerful operando techniques for the study of active sites is near ambient pressure X-ray photoelectron spectroscopy (NAP-XPS), which is particularly sensitive to the surface and sub-surface of solids. Here we review the use of NAP-XPS for the study of ceria-based catalysts, widely used in a large number of industrial processes due to their excellent oxygen storage capacity and well-established redox properties.

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“…[1][2][3] In addition to being combusted with O2as a source in the production of electricity or heat, natural gas and biogas can also be used as chemical feedstock in the manufacture of commodity chemicals, and this is achieved indirectly by reforming CH4 to syngas (H2 and CO) and subsequently converting syngas to upgraded chemicals. [4][5] There are three oxidative pathways to produce syngas from methane: (1) partial oxidation, (2) steam reforming and (3) dry reforming:…”

Section: Introductionmentioning

confidence: 99%

In Situ Elucidation of the Active State of Co–CeO_x Catalysts in the Dry Reforming of Methane: The Important Role of the Reducible Oxide Support and Interactions with Cobalt

et al. 2018

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The dry reforming of methane was systematically studied over a series (2-30 wt%) of Co (~5nm in size) loaded CeO2 catalysts, with an effort to elucidate the behavior of Co and ceria in the catalytic process using in-situ methods. For the systems under study, the reaction activity scaled with increasing Co loading, and a 10 wt% Co-CeO2 catalyst exhibiting the best catalytic activity and good stability at 500 °C with little evidence for carbon accumulation. The phase transitions and the nature of active components in the catalyst were investigated during pretreatment and under reaction conditions by ex-situ/in-situ techniques including X-ray diffraction (XRD) and ambient-pressure X-ray photoelectron spectroscopy (AP-XPS). These studies showed a dynamical evolution in the chemical composition of the catalysts under reaction conditions. A clear transition of Co3O4 → CoO → Co, and Ce 4+ to Ce 3+ , was observed during the temperature programmed reduction under H2 and CH4. However, introduction of CO2, led to partial re-oxidation of all components at low temperatures, followed by reduction at high temperatures. Under optimum CO and H2 producing conditions both XRD and AP-XPS indicated that the active phase involved a majority of metallic Co with a small amount of CoO both supported on a partially reduced ceria (Ce 3+ /Ce 4+). We identified the importance of dispersing Co, anchoring it onto ceria surface sites, and then utilizing the redox properties of ceria for activating and then oxidatively converting methane while inhibiting coke formation. Furthermore, a synergistic effect between cobalt and ceria and the interfacial site are essential to successfully close the catalytic cycle.

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High energy efficiency in syngas and hydrocarbon production from dissociation of CH₄–CO₂mixture in a non-equilibrium pulsed plasma

Cited by 37 publications

References 28 publications

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

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

Ceria-Based Catalysts Studied by Near Ambient Pressure X-ray Photoelectron Spectroscopy: A Review

In Situ Elucidation of the Active State of Co–CeO_x Catalysts in the Dry Reforming of Methane: The Important Role of the Reducible Oxide Support and Interactions with Cobalt

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High energy efficiency in syngas and hydrocarbon production from dissociation of CH4–CO2mixture in a non-equilibrium pulsed plasma

Cited by 37 publications

References 28 publications

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

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

Ceria-Based Catalysts Studied by Near Ambient Pressure X-ray Photoelectron Spectroscopy: A Review

In Situ Elucidation of the Active State of Co–CeOx Catalysts in the Dry Reforming of Methane: The Important Role of the Reducible Oxide Support and Interactions with Cobalt

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High energy efficiency in syngas and hydrocarbon production from dissociation of CH₄–CO₂mixture in a non-equilibrium pulsed plasma

In Situ Elucidation of the Active State of Co–CeO_x Catalysts in the Dry Reforming of Methane: The Important Role of the Reducible Oxide Support and Interactions with Cobalt