Enabling complete conversion of CH4 and CO2 in dynamic coke-mediated dry reforming (DC-DRM) on Ni catalysts

Donato Pinto; Lingjun Hu; Atsushi Urakawa

doi:10.1016/j.cej.2023.145641

Enabling complete conversion of CH₄ and CO₂ in dynamic coke-mediated dry reforming (DC-DRM) on Ni catalysts

Donato Pinto, Lingjun Hu, Atsushi Urakawa^*

^*Corresponding author for this work

ChemE/Catalysis Engineering

Research output: Contribution to journal › Article › Scientific › peer-review

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Abstract

Dynamic coke-mediated dry reforming of methane (DC-DRM) is an unsteady-state strategy to overcome the limitations of co-feed operation, including the fast deactivation of the catalysts and the loss of valuable H₂ in the reverse water gas-shift reaction. This paper proves the feasibility of DC-DRM on Ni-based catalytic systems, identifying suitable metal oxides supports and evaluating the role of metallic promoters. A La-promoted Ni/ZrO₂ catalyst exhibited excellent and stable catalytic performances at 800 °C approaching complete conversion of the CH₄ and CO₂ reactant pulses in the reaction loop, and separation of the H₂ and CO product streams. Adding the redox functionality of reducible oxides (TiO₂) in the catalyst support is demonstrated as a powerful tool to enable direct formation of syngas in the methane pulse with control on the H₂/CO ratio.

Original language	English
Article number	145641
Number of pages	12
Journal	Chemical Engineering Journal
Volume	474
DOIs	https://doi.org/10.1016/j.cej.2023.145641
Publication status	Published - 2023

Keywords

CH dry reforming
CO conversion
Heterogeneous catalysis
Ni catalysts
Unsteady-state

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10.1016/j.cej.2023.145641

1-s2.0-S1385894723043723-mainFinal published version, 6.15 MBLicence: CC BY

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title = "Enabling complete conversion of CH4 and CO2 in dynamic coke-mediated dry reforming (DC-DRM) on Ni catalysts",

abstract = "Dynamic coke-mediated dry reforming of methane (DC-DRM) is an unsteady-state strategy to overcome the limitations of co-feed operation, including the fast deactivation of the catalysts and the loss of valuable H2 in the reverse water gas-shift reaction. This paper proves the feasibility of DC-DRM on Ni-based catalytic systems, identifying suitable metal oxides supports and evaluating the role of metallic promoters. A La-promoted Ni/ZrO2 catalyst exhibited excellent and stable catalytic performances at 800 °C approaching complete conversion of the CH4 and CO2 reactant pulses in the reaction loop, and separation of the H2 and CO product streams. Adding the redox functionality of reducible oxides (TiO2) in the catalyst support is demonstrated as a powerful tool to enable direct formation of syngas in the methane pulse with control on the H2/CO ratio.",

keywords = "CH dry reforming, CO conversion, Heterogeneous catalysis, Ni catalysts, Unsteady-state",

author = "Donato Pinto and Lingjun Hu and Atsushi Urakawa",

year = "2023",

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language = "English",

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journal = "Chemical Engineering Journal",

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T1 - Enabling complete conversion of CH4 and CO2 in dynamic coke-mediated dry reforming (DC-DRM) on Ni catalysts

AU - Pinto, Donato

AU - Hu, Lingjun

AU - Urakawa, Atsushi

PY - 2023

Y1 - 2023

N2 - Dynamic coke-mediated dry reforming of methane (DC-DRM) is an unsteady-state strategy to overcome the limitations of co-feed operation, including the fast deactivation of the catalysts and the loss of valuable H2 in the reverse water gas-shift reaction. This paper proves the feasibility of DC-DRM on Ni-based catalytic systems, identifying suitable metal oxides supports and evaluating the role of metallic promoters. A La-promoted Ni/ZrO2 catalyst exhibited excellent and stable catalytic performances at 800 °C approaching complete conversion of the CH4 and CO2 reactant pulses in the reaction loop, and separation of the H2 and CO product streams. Adding the redox functionality of reducible oxides (TiO2) in the catalyst support is demonstrated as a powerful tool to enable direct formation of syngas in the methane pulse with control on the H2/CO ratio.

AB - Dynamic coke-mediated dry reforming of methane (DC-DRM) is an unsteady-state strategy to overcome the limitations of co-feed operation, including the fast deactivation of the catalysts and the loss of valuable H2 in the reverse water gas-shift reaction. This paper proves the feasibility of DC-DRM on Ni-based catalytic systems, identifying suitable metal oxides supports and evaluating the role of metallic promoters. A La-promoted Ni/ZrO2 catalyst exhibited excellent and stable catalytic performances at 800 °C approaching complete conversion of the CH4 and CO2 reactant pulses in the reaction loop, and separation of the H2 and CO product streams. Adding the redox functionality of reducible oxides (TiO2) in the catalyst support is demonstrated as a powerful tool to enable direct formation of syngas in the methane pulse with control on the H2/CO ratio.

KW - CH dry reforming

KW - CO conversion

KW - Heterogeneous catalysis

KW - Ni catalysts

KW - Unsteady-state

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Enabling complete conversion of CH₄ and CO₂ in dynamic coke-mediated dry reforming (DC-DRM) on Ni catalysts

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