Utilization of CO2 in non-catalytic dry reforming of C1–C4 hydrocarbons

Савченко, В. И.; Zimin, Ya. S.; Никитин, А. В.; Седов, И. В.; Arutyunov, V. S.

doi:10.1016/j.jcou.2021.101490

Cited by 28 publications

(13 citation statements)

References 34 publications

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“…A slight, at a ~4 kJ/mol level, difference is most likely associated with certain arbitrariness in selection of the specific approximating expressions for describing the calculated results and is hardly interpretable as really meaningful. Thus, our results may be considered as a kinetic evidence validating the assumption made in [14,15] that, in the temperature range 1400-1800 K, all the studied methane conversion processes involve the thermal pyrolysis stage.…”

Section: Modeling the Methane Conversion Processessupporting

confidence: 87%

“…Previously [14,15], we made an assumption that steam reforming and carbon dioxide reforming of methane proceed via its preliminary thermal pyrolysis to acetylene, which conclusion was further extended to incorporate higher homologs of methane [15,20]. For validation of this conclusion, we compared in this study the kinetics of conversion of methane in the processes of steam and carbon dioxide reforming with that of its conversion in thermal pyrolysis.…”

Section: Modeling the Methane Conversion Processesmentioning

confidence: 99%

“…At least, we could not find meaningful works on the kinetics of these processes in the range of conditions considered. Earlier, we carried out the kinetic analysis of steam reforming [14] and carbon dioxide reforming [15] of methane and showed that, in both cases, the methane conversion and hydrogen formation began at a much earlier point of time than the conversion of Н 2 О and СО 2 , respectively (Fig. 1).…”

mentioning

confidence: 92%

“…Noticeable conversion of water vapor and carbon dioxide began only after appearance of acetylene among the reaction products (Fig. 1) and resulted from their interaction with the H • atoms yielded by methane pyrolysis and the subsequent reaction of OH • radicals with acetylene [15].…”

mentioning

confidence: 99%

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On the Mechanism of Methane Conversion in the Nonсatalytic Processes of Its Thermal Pyrolysis and Steam and Carbon Dioxide Reforming

2021

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A detailed kinetic modeling of the noncatalytic processes of thermal pyrolysis and steam and carbon dioxide reforming of methane revealed almost completely identical kinetics of the methane conversion in these processes. This suggests that, in the temperature range 1400–1800 K, the initial stage of conversion of methane in all these processes is its thermal pyrolysis. The modeling results agree well with the experimental data on methane pyrolysis. For the temperature range examined, the Arrhenius expressions (pre-exponential factors and activation energy) were obtained in the first-order kinetics approximation for the rate of methane conversion in the processes studied. The expressions derived may be useful for making preliminary estimates and carrying out engineering calculations.

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Section: Modeling the Methane Conversion Processessupporting

confidence: 87%

Section: Modeling the Methane Conversion Processesmentioning

confidence: 99%

mentioning

confidence: 92%

mentioning

confidence: 99%

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On the Mechanism of Methane Conversion in the Nonсatalytic Processes of Its Thermal Pyrolysis and Steam and Carbon Dioxide Reforming

2021

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“…As a consequence, CO 2 promotes the formation of OH radicals in the dry reforming of methane, thereby, increasing the reactivity of the primary reaction pathway (reaction ( 7)) for C2 formation [36]. The decline in CO 2 mole fraction along with rise in C 2 H 2 is more profound in the case of a CH 4 /O 2 of 1.4, as compared with CH 4 /O 2 of 1.6 (Figure 10).…”

Section: Homogeneous Reaction Kinetics After the Monolithmentioning

confidence: 99%

Oxidative Coupling of Methane over Pt/Al2O3 at High Temperature: Multiscale Modeling of the Catalytic Monolith

et al. 2022

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At high temperatures, the oxidative coupling of methane (OCM) is an attractive approach for catalytic conversion of methane into value-added chemicals. Experiments with a Pt/Al2O3-coated catalytic honeycomb monolith were conducted with varying CH4/O2 ratios, N2 dilution at atmospheric pressure, and very short contact times. The reactor was modeled by a multiscale approach using a parabolic two-dimensional flow field description in the monolithic channels coupled with a heat balance of the monolithic structure, and multistep surface reaction mechanisms as well as elementary-step, gas phase reaction mechanisms. The contribution of heterogeneous and homogeneous reactions, both of which are important for the optimization of C2 products, is investigated using a combination of experimental and computational methods. The oxidation of methane, which takes place over the platinum catalyst, causes the adiabatic temperature increase required for the generation of CH3 radicals in the gas phase, which are essential for the formation of C2 species. Lower CH4/O2 ratios result in higher C2 selectivity. However, the presence of OH radicals at high temperatures facilitates subsequent conversion of C2H2 at a CH4/O2 ratio of 1.4. Thereby, C2 species selectivity of 7% was achieved at CH4/O2 ratio of 1.6, with 35% N2 dilution.

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A Carbon Capture and Utilization Process for the Production of Solid Carbon Materials from Atmospheric CO₂ – Part 1: Process Performance

Uhlenbruck,

Pfeifer,

Dietrich

et al. 2024

ChemSusChem

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The successful operation of a process that converts atmospheric CO2 into solid carbon products is presented as an alternative to fossil based solid carbon production. In a first step, CO2 is removed from the atmosphere by a direct air capture (DAC) unit. The gas is then mixed with hydrogen and enters a methanation unit. Depending on the operation conditions, gas mixtures consisting of mainly methane with either H2 or CO2 as side‐component are obtained. After precipitating the water formed during the methanation step, the remaining gas mixture is fed into a bubble column reactor filled with liquid tin. During the rise of the gas bubbles, methane is thermally split up into hydrogen and solid carbon. The latter is continuously removed from the liquid metal surface as a fine powder by pneumatic conveying. This article is the first of two articles, focusing on the performance of the methanation and methane pyrolysis steps. The experimental results are complemented by thermodynamic analyses and reaction modelling. A detailed analysis of the solid carbon product of the process is presented in the second part.

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Utilization of CO2 in non-catalytic dry reforming of C1–C4 hydrocarbons

Cited by 28 publications

References 34 publications

On the Mechanism of Methane Conversion in the Nonсatalytic Processes of Its Thermal Pyrolysis and Steam and Carbon Dioxide Reforming

On the Mechanism of Methane Conversion in the Nonсatalytic Processes of Its Thermal Pyrolysis and Steam and Carbon Dioxide Reforming

Oxidative Coupling of Methane over Pt/Al2O3 at High Temperature: Multiscale Modeling of the Catalytic Monolith

A Carbon Capture and Utilization Process for the Production of Solid Carbon Materials from Atmospheric CO₂ – Part 1: Process Performance

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Utilization of CO2 in non-catalytic dry reforming of C1–C4 hydrocarbons

Cited by 28 publications

References 34 publications

On the Mechanism of Methane Conversion in the Nonсatalytic Processes of Its Thermal Pyrolysis and Steam and Carbon Dioxide Reforming

On the Mechanism of Methane Conversion in the Nonсatalytic Processes of Its Thermal Pyrolysis and Steam and Carbon Dioxide Reforming

Oxidative Coupling of Methane over Pt/Al2O3 at High Temperature: Multiscale Modeling of the Catalytic Monolith

A Carbon Capture and Utilization Process for the Production of Solid Carbon Materials from Atmospheric CO2 – Part 1: Process Performance

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A Carbon Capture and Utilization Process for the Production of Solid Carbon Materials from Atmospheric CO₂ – Part 1: Process Performance