Uncovering the reaction mechanism behind CoO as active phase for CO2 hydrogenation

Transforming carbon dioxide into valuable chemicals and fuels, is a promising tool for environmental and industrial purposes. Here, we present catalysts comprising of cobalt (oxide) nanoparticles stabilized on various support oxides for hydrocarbon production from carbon dioxide. We demonstrate that...

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Vydané v:Nature communications Ročník 13; číslo 1; s. 324 - 11
Hlavní autori: Have, Iris C. ten, Kromwijk, Josepha J. G., Monai, Matteo, Ferri, Davide, Sterk, Ellen B., Meirer, Florian, Weckhuysen, Bert M.
Médium: Journal Article
Jazyk:English
Vydavateľské údaje: London Nature Publishing Group UK 14.01.2022
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ISSN:2041-1723, 2041-1723
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Abstract Transforming carbon dioxide into valuable chemicals and fuels, is a promising tool for environmental and industrial purposes. Here, we present catalysts comprising of cobalt (oxide) nanoparticles stabilized on various support oxides for hydrocarbon production from carbon dioxide. We demonstrate that the activity and selectivity can be tuned by selection of the support oxide and cobalt oxidation state. Modulated excitation (ME) diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) reveals that cobalt oxide catalysts follows the hydrogen-assisted pathway, whereas metallic cobalt catalysts mainly follows the direct dissociation pathway. Contrary to the commonly considered metallic active phase of cobalt-based catalysts, cobalt oxide on titania support is the most active catalyst in this study and produces 11% C 2+ hydrocarbons. The C 2+ selectivity increases to 39% (yielding 104 mmol h −1  g cat −1 C 2+ hydrocarbons) upon co-feeding CO and CO 2 at a ratio of 1:2 at 250 °C and 20 bar, thus outperforming the majority of typical cobalt-based catalysts. Catalytic conversion of CO 2 into valuable hydrocarbons is a promising way to mitigate climate change. This work uncovers that cobalt oxide nanoparticles on a titania carrier produce more C 2+ hydrocarbons than their metallic cobalt counterpart by following a different reaction mechanism.
AbstractList Transforming carbon dioxide into valuable chemicals and fuels, is a promising tool for environmental and industrial purposes. Here, we present catalysts comprising of cobalt (oxide) nanoparticles stabilized on various support oxides for hydrocarbon production from carbon dioxide. We demonstrate that the activity and selectivity can be tuned by selection of the support oxide and cobalt oxidation state. Modulated excitation (ME) diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) reveals that cobalt oxide catalysts follows the hydrogen-assisted pathway, whereas metallic cobalt catalysts mainly follows the direct dissociation pathway. Contrary to the commonly considered metallic active phase of cobalt-based catalysts, cobalt oxide on titania support is the most active catalyst in this study and produces 11% C2+ hydrocarbons. The C2+ selectivity increases to 39% (yielding 104 mmol h−1 gcat−1 C2+ hydrocarbons) upon co-feeding CO and CO2 at a ratio of 1:2 at 250 °C and 20 bar, thus outperforming the majority of typical cobalt-based catalysts. Catalytic conversion of CO2 into valuable hydrocarbons is a promising way to mitigate climate change. This work uncovers that cobalt oxide nanoparticles on a titania carrier produce more C2+ hydrocarbons than their metallic cobalt counterpart by following a different reaction mechanism.
Transforming carbon dioxide into valuable chemicals and fuels, is a promising tool for environmental and industrial purposes. Here, we present catalysts comprising of cobalt (oxide) nanoparticles stabilized on various support oxides for hydrocarbon production from carbon dioxide. We demonstrate that the activity and selectivity can be tuned by selection of the support oxide and cobalt oxidation state. Modulated excitation (ME) diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) reveals that cobalt oxide catalysts follows the hydrogen-assisted pathway, whereas metallic cobalt catalysts mainly follows the direct dissociation pathway. Contrary to the commonly considered metallic active phase of cobalt-based catalysts, cobalt oxide on titania support is the most active catalyst in this study and produces 11% C 2+ hydrocarbons. The C 2+ selectivity increases to 39% (yielding 104 mmol h −1  g cat −1 C 2+ hydrocarbons) upon co-feeding CO and CO 2 at a ratio of 1:2 at 250 °C and 20 bar, thus outperforming the majority of typical cobalt-based catalysts. Catalytic conversion of CO 2 into valuable hydrocarbons is a promising way to mitigate climate change. This work uncovers that cobalt oxide nanoparticles on a titania carrier produce more C 2+ hydrocarbons than their metallic cobalt counterpart by following a different reaction mechanism.
Transforming carbon dioxide into valuable chemicals and fuels, is a promising tool for environmental and industrial purposes. Here, we present catalysts comprising of cobalt (oxide) nanoparticles stabilized on various support oxides for hydrocarbon production from carbon dioxide. We demonstrate that the activity and selectivity can be tuned by selection of the support oxide and cobalt oxidation state. Modulated excitation (ME) diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) reveals that cobalt oxide catalysts follows the hydrogen-assisted pathway, whereas metallic cobalt catalysts mainly follows the direct dissociation pathway. Contrary to the commonly considered metallic active phase of cobalt-based catalysts, cobalt oxide on titania support is the most active catalyst in this study and produces 11% C2+ hydrocarbons. The C2+ selectivity increases to 39% (yielding 104 mmol h-1 gcat-1 C2+ hydrocarbons) upon co-feeding CO and CO2 at a ratio of 1:2 at 250 °C and 20 bar, thus outperforming the majority of typical cobalt-based catalysts.Transforming carbon dioxide into valuable chemicals and fuels, is a promising tool for environmental and industrial purposes. Here, we present catalysts comprising of cobalt (oxide) nanoparticles stabilized on various support oxides for hydrocarbon production from carbon dioxide. We demonstrate that the activity and selectivity can be tuned by selection of the support oxide and cobalt oxidation state. Modulated excitation (ME) diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) reveals that cobalt oxide catalysts follows the hydrogen-assisted pathway, whereas metallic cobalt catalysts mainly follows the direct dissociation pathway. Contrary to the commonly considered metallic active phase of cobalt-based catalysts, cobalt oxide on titania support is the most active catalyst in this study and produces 11% C2+ hydrocarbons. The C2+ selectivity increases to 39% (yielding 104 mmol h-1 gcat-1 C2+ hydrocarbons) upon co-feeding CO and CO2 at a ratio of 1:2 at 250 °C and 20 bar, thus outperforming the majority of typical cobalt-based catalysts.
Transforming carbon dioxide into valuable chemicals and fuels, is a promising tool for environmental and industrial purposes. Here, we present catalysts comprising of cobalt (oxide) nanoparticles stabilized on various support oxides for hydrocarbon production from carbon dioxide. We demonstrate that the activity and selectivity can be tuned by selection of the support oxide and cobalt oxidation state. Modulated excitation (ME) diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) reveals that cobalt oxide catalysts follows the hydrogen-assisted pathway, whereas metallic cobalt catalysts mainly follows the direct dissociation pathway. Contrary to the commonly considered metallic active phase of cobalt-based catalysts, cobalt oxide on titania support is the most active catalyst in this study and produces 11% C 2+ hydrocarbons. The C 2+ selectivity increases to 39% (yielding 104 mmol h −1  g cat −1 C 2+ hydrocarbons) upon co-feeding CO and CO 2 at a ratio of 1:2 at 250 °C and 20 bar, thus outperforming the majority of typical cobalt-based catalysts.
Catalytic conversion of CO2 into valuable hydrocarbons is a promising way to mitigate climate change. This work uncovers that cobalt oxide nanoparticles on a titania carrier produce more C2+ hydrocarbons than their metallic cobalt counterpart by following a different reaction mechanism.
ArticleNumber 324
Author Monai, Matteo
Kromwijk, Josepha J. G.
Ferri, Davide
Have, Iris C. ten
Weckhuysen, Bert M.
Meirer, Florian
Sterk, Ellen B.
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  publication-title: Nat. Commun.
  doi: 10.1038/s41467-020-14817-9
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  doi: 10.1021/acs.chemrev.8b00705
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  publication-title: Rev. Sci. Instrum.
  doi: 10.1063/1.4890668
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Snippet Transforming carbon dioxide into valuable chemicals and fuels, is a promising tool for environmental and industrial purposes. Here, we present catalysts...
Catalytic conversion of CO2 into valuable hydrocarbons is a promising way to mitigate climate change. This work uncovers that cobalt oxide nanoparticles on a...
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SubjectTerms 119/118
140/146
639/638/77/885
639/638/77/887
704/172/169/896
Carbon dioxide
Catalysts
Catalytic converters
Climate change
Climate change mitigation
Cobalt
Cobalt oxides
Fourier transforms
Humanities and Social Sciences
Hydrocarbons
multidisciplinary
Nanoparticles
Oxidation
Reaction mechanisms
Science
Science (multidisciplinary)
Selectivity
Titanium dioxide
Valence
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Title Uncovering the reaction mechanism behind CoO as active phase for CO2 hydrogenation
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