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Investigation dry reforming of methane over nickel using a one‐dimensional model

  • In the field of catalysis, dry reforming, that is, methane reforming with CO2, is in the focus due to growing environmental concerns about oil depletion and global warming with a desire to produce synthesis gas. However, this process can lead to the formation of carbon, which can cause catalyst deactivation, especially at industrial conditions. Nevertheless, the key to develop a more coke-resistant catalyst is a better comprehension of the reforming process at a molecular level. Regardless of all the investigations available in literature, the detailed path for the conversion of methane to syngas and carbon remains a controversial issue. Another problem in setting up a reaction mechanism is the difficulty to define the thermodynamic data for intermediate surface species and this leads to the development of thermodynamic consistent surface reaction mechanisms in literature where the thermodynamic data are not used to calculate the rate coefficients of the reverse reactions. Rather the Arrhenius parameters for the forward as well asIn the field of catalysis, dry reforming, that is, methane reforming with CO2, is in the focus due to growing environmental concerns about oil depletion and global warming with a desire to produce synthesis gas. However, this process can lead to the formation of carbon, which can cause catalyst deactivation, especially at industrial conditions. Nevertheless, the key to develop a more coke-resistant catalyst is a better comprehension of the reforming process at a molecular level. Regardless of all the investigations available in literature, the detailed path for the conversion of methane to syngas and carbon remains a controversial issue. Another problem in setting up a reaction mechanism is the difficulty to define the thermodynamic data for intermediate surface species and this leads to the development of thermodynamic consistent surface reaction mechanisms in literature where the thermodynamic data are not used to calculate the rate coefficients of the reverse reactions. Rather the Arrhenius parameters for the forward as well as backward reactions are explicitly given in the reaction mechanism to establish thermodynamic equilibrium. In this investigation, a kinetically consistent detailed surface reaction mechanism is developed which consists of 26 reversible reactions with the help of a one-dimensional model, LOGEcat. Our previous work constructs the basis of the present investigation. Further, a detailed sensitivity analysis of reversible reactions and reaction pathways is performed to understand the mechanism better. The mechanism is validated for dry reforming of methane over nickel catalyst, however, it can also be used for other processes, such as, steam reforming and partial oxidation. The mechanism is tested by comparing the simulation results with the literature experiments and simulations in a wide range of temperature. The new developed kinetically consistent surface reaction mechanism is able to accurately express the dry reforming of methane over the nickel catalyst for complete range of temperature and also provide a useful insight into the key rate determining steps.show moreshow less

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Author: Rakhi RakhiORCiD, Binod Raj GiriORCiD, Vivien GüntherORCiD, Fabian MaussORCiD
URL:https://onlinelibrary.wiley.com/doi/pdf/10.1002/pamm.202300266
DOI:https://doi.org/10.1002/pamm.202300266
Title of the source (English):PAMM
Document Type:Conference publication peer-reviewed
Language:English
Year of publication:2023
Volume/Year:23
Issue number:4
Number of pages:8
Faculty/Chair:Fakultät 3 Maschinenbau, Elektro- und Energiesysteme / FG Thermodynamik / Thermische Verfahrenstechnik
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