Ceria-Supported Cobalt Catalyst for Low-Temperature Methanation at Low Partial Pressures of CO2

Job J.C. Struijs; Valery Muravev; Marcel A. Verheijen; Emiel J.M. Hensen; Nikolay Kosinov

doi:10.1002/anie.202214864

Ceria-Supported Cobalt Catalyst for Low-Temperature Methanation at Low Partial Pressures of CO₂

Job J.C. Struijs, Valery Muravev, Marcel A. Verheijen, Emiel J.M. Hensen (Corresponding author), Nikolay Kosinov (Corresponding author)

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

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Abstract

The direct catalytic conversion of atmospheric CO₂ to valuable chemicals is a promising solution to avert negative consequences of rising CO₂ concentration. However, heterogeneous catalysts efficient at low partial pressures of CO₂ still need to be developed. Here, we explore Co/CeO₂ as a catalyst for the methanation of diluted CO₂ streams. This material displays an excellent performance at reaction temperatures as low as 175 °C and CO₂ partial pressures as low as 0.4 mbar (the atmospheric CO₂ concentration). To gain mechanistic understanding of this unusual activity, we employed in situ X-ray photoelectron spectroscopy and operando infrared spectroscopy. The higher surface concentration and reactivity of formates and carbonyls—key reaction intermediates—explain the superior activity of Co/CeO₂ as compared to a conventional Co/SiO₂ catalyst. This work emphasizes the catalytic role of the cobalt-ceria interface and will aid in developing more efficient CO₂ hydrogenation catalysts.

Original language	English
Article number	e202214864
Number of pages	9
Journal	Angewandte Chemie - International Edition
Volume	62
Issue number	5
DOIs	https://doi.org/10.1002/anie.202214864
Publication status	Published - 26 Jan 2023

Bibliographical note

Funding Information:
This publication is part of the project OCENW.XS3.007 which is financed by the Dutch Research Council (NWO). Solliance and the Dutch Province of Noord‐Brabant are acknowledged for funding the TEM facility. The authors thank dr. Alexander Parastaev for his assistance with experiments and the fruitful discussions.

Funding

This publication is part of the project OCENW.XS3.007 which is financed by the Dutch Research Council (NWO). Solliance and the Dutch Province of Noord‐Brabant are acknowledged for funding the TEM facility. The authors thank dr. Alexander Parastaev for his assistance with experiments and the fruitful discussions.

Keywords

Atmospheric CO Valorization
Ceria
CO Hydrogenation
Cobalt
Reaction Mechanisms

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Cite this

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title = "Ceria-Supported Cobalt Catalyst for Low-Temperature Methanation at Low Partial Pressures of CO2",

abstract = "The direct catalytic conversion of atmospheric CO2 to valuable chemicals is a promising solution to avert negative consequences of rising CO2 concentration. However, heterogeneous catalysts efficient at low partial pressures of CO2 still need to be developed. Here, we explore Co/CeO2 as a catalyst for the methanation of diluted CO2 streams. This material displays an excellent performance at reaction temperatures as low as 175 °C and CO2 partial pressures as low as 0.4 mbar (the atmospheric CO2 concentration). To gain mechanistic understanding of this unusual activity, we employed in situ X-ray photoelectron spectroscopy and operando infrared spectroscopy. The higher surface concentration and reactivity of formates and carbonyls—key reaction intermediates—explain the superior activity of Co/CeO2 as compared to a conventional Co/SiO2 catalyst. This work emphasizes the catalytic role of the cobalt-ceria interface and will aid in developing more efficient CO2 hydrogenation catalysts.",

keywords = "Atmospheric CO Valorization, Ceria, CO Hydrogenation, Cobalt, Reaction Mechanisms",

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note = "Funding Information: This publication is part of the project OCENW.XS3.007 which is financed by the Dutch Research Council (NWO). Solliance and the Dutch Province of Noord‐Brabant are acknowledged for funding the TEM facility. The authors thank dr. Alexander Parastaev for his assistance with experiments and the fruitful discussions. ",

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AU - Hensen, Emiel J.M.

AU - Kosinov, Nikolay

N1 - Funding Information: This publication is part of the project OCENW.XS3.007 which is financed by the Dutch Research Council (NWO). Solliance and the Dutch Province of Noord‐Brabant are acknowledged for funding the TEM facility. The authors thank dr. Alexander Parastaev for his assistance with experiments and the fruitful discussions.

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N2 - The direct catalytic conversion of atmospheric CO2 to valuable chemicals is a promising solution to avert negative consequences of rising CO2 concentration. However, heterogeneous catalysts efficient at low partial pressures of CO2 still need to be developed. Here, we explore Co/CeO2 as a catalyst for the methanation of diluted CO2 streams. This material displays an excellent performance at reaction temperatures as low as 175 °C and CO2 partial pressures as low as 0.4 mbar (the atmospheric CO2 concentration). To gain mechanistic understanding of this unusual activity, we employed in situ X-ray photoelectron spectroscopy and operando infrared spectroscopy. The higher surface concentration and reactivity of formates and carbonyls—key reaction intermediates—explain the superior activity of Co/CeO2 as compared to a conventional Co/SiO2 catalyst. This work emphasizes the catalytic role of the cobalt-ceria interface and will aid in developing more efficient CO2 hydrogenation catalysts.

AB - The direct catalytic conversion of atmospheric CO2 to valuable chemicals is a promising solution to avert negative consequences of rising CO2 concentration. However, heterogeneous catalysts efficient at low partial pressures of CO2 still need to be developed. Here, we explore Co/CeO2 as a catalyst for the methanation of diluted CO2 streams. This material displays an excellent performance at reaction temperatures as low as 175 °C and CO2 partial pressures as low as 0.4 mbar (the atmospheric CO2 concentration). To gain mechanistic understanding of this unusual activity, we employed in situ X-ray photoelectron spectroscopy and operando infrared spectroscopy. The higher surface concentration and reactivity of formates and carbonyls—key reaction intermediates—explain the superior activity of Co/CeO2 as compared to a conventional Co/SiO2 catalyst. This work emphasizes the catalytic role of the cobalt-ceria interface and will aid in developing more efficient CO2 hydrogenation catalysts.

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