Probing the Reactive Intermediates in CO2 Hydrogenation on Ni/Al2O3 Catalysts with Modulation Excitation Spectroscopy.
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| Title: | Probing the Reactive Intermediates in CO |
|---|---|
| Authors: | Kock, Mikkel1 (AUTHOR), Kowalewski, Emil1 (AUTHOR), Iltsiou, Dimitra1 (AUTHOR), Mielby, Jerrik1 (AUTHOR) jjmie@kemi.dtu.dk, Kegnæs, Søren1 (AUTHOR) skk@kemi.dtu.dk |
| Source: | ChemCatChem. 2/22/2024, Vol. 16 Issue 4, p1-9. 9p. |
| Subjects: | Modulation spectroscopy, Fourier transform infrared spectroscopy, Catalysts, Catalyst supports, Catalytic activity |
| Abstract: | In‐situ infrared spectroscopy is one of the most effective methods to study the surface species on solid catalysts. Still, it is sometimes difficult to identify the reactive intermediates because spectator species, the catalyst support, and experimental noise also contribute to the total spectra. In this study, we prepared three archetypical Ni/Al2O3 catalysts that showed significantly different catalytic activity and selectivity for CO2 hydrogenation, depending on the calcination and reduction temperature. After detailed characterization, we used a combination of Modulation Excitation‐Phase Sensitive Detection‐Diffuse Reflectance Infrared Fourier Transform Spectroscopy (ME‐PSD‐DRIFTS) and Steady State Isotopic Kinetic Analysis (SSITKA) to show that bicarbonates and formates are key reactive intermediates. Furthermore, we also observe carbonyls on the catalyst with the most metallic character and highest selectivity towards CH4. These results confirm that the hydrogenation of CO2 occurs in an associative and consecutive reaction pathway that is highly structure‐sensitive. In this way, we also demonstrate how the simultaneous collection of spectroscopic and kinetic data during modulated or transient experiments is a powerful tool for investigating solid catalysts under realistic operation conditions. [ABSTRACT FROM AUTHOR] |
| Copyright of ChemCatChem is the property of Wiley-Blackwell and its content may not be copied or emailed to multiple sites without the copyright holder's express written permission. Additionally, content may not be used with any artificial intelligence tools or machine learning technologies. However, users may print, download, or email articles for individual use. This abstract may be abridged. No warranty is given about the accuracy of the copy. Users should refer to the original published version of the material for the full abstract. (Copyright applies to all Abstracts.) | |
| Database: | Engineering Source |
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| Header | DbId: egs DbLabel: Engineering Source An: 175640651 AccessLevel: 6 PubType: Academic Journal PubTypeId: academicJournal PreciseRelevancyScore: 0 |
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| Items | – Name: Title Label: Title Group: Ti Data: Probing the Reactive Intermediates in CO<subscript>2</subscript> Hydrogenation on Ni/Al<subscript>2</subscript>O<subscript>3</subscript> Catalysts with Modulation Excitation Spectroscopy. – Name: Author Label: Authors Group: Au Data: <searchLink fieldCode="AR" term="%22Kock%2C+Mikkel%22">Kock, Mikkel</searchLink><relatesTo>1</relatesTo> (AUTHOR)<br /><searchLink fieldCode="AR" term="%22Kowalewski%2C+Emil%22">Kowalewski, Emil</searchLink><relatesTo>1</relatesTo> (AUTHOR)<br /><searchLink fieldCode="AR" term="%22Iltsiou%2C+Dimitra%22">Iltsiou, Dimitra</searchLink><relatesTo>1</relatesTo> (AUTHOR)<br /><searchLink fieldCode="AR" term="%22Mielby%2C+Jerrik%22">Mielby, Jerrik</searchLink><relatesTo>1</relatesTo> (AUTHOR)<i> jjmie@kemi.dtu.dk</i><br /><searchLink fieldCode="AR" term="%22Kegnæs%2C+Søren%22">Kegnæs, Søren</searchLink><relatesTo>1</relatesTo> (AUTHOR)<i> skk@kemi.dtu.dk</i> – Name: TitleSource Label: Source Group: Src Data: <searchLink fieldCode="JN" term="%22ChemCatChem%22">ChemCatChem</searchLink>. 2/22/2024, Vol. 16 Issue 4, p1-9. 9p. – Name: Subject Label: Subjects Group: Su Data: <searchLink fieldCode="DE" term="%22Modulation+spectroscopy%22">Modulation spectroscopy</searchLink><br /><searchLink fieldCode="DE" term="%22Fourier+transform+infrared+spectroscopy%22">Fourier transform infrared spectroscopy</searchLink><br /><searchLink fieldCode="DE" term="%22Catalysts%22">Catalysts</searchLink><br /><searchLink fieldCode="DE" term="%22Catalyst+supports%22">Catalyst supports</searchLink><br /><searchLink fieldCode="DE" term="%22Catalytic+activity%22">Catalytic activity</searchLink> – Name: Abstract Label: Abstract Group: Ab Data: In‐situ infrared spectroscopy is one of the most effective methods to study the surface species on solid catalysts. Still, it is sometimes difficult to identify the reactive intermediates because spectator species, the catalyst support, and experimental noise also contribute to the total spectra. In this study, we prepared three archetypical Ni/Al2O3 catalysts that showed significantly different catalytic activity and selectivity for CO2 hydrogenation, depending on the calcination and reduction temperature. After detailed characterization, we used a combination of Modulation Excitation‐Phase Sensitive Detection‐Diffuse Reflectance Infrared Fourier Transform Spectroscopy (ME‐PSD‐DRIFTS) and Steady State Isotopic Kinetic Analysis (SSITKA) to show that bicarbonates and formates are key reactive intermediates. Furthermore, we also observe carbonyls on the catalyst with the most metallic character and highest selectivity towards CH4. These results confirm that the hydrogenation of CO2 occurs in an associative and consecutive reaction pathway that is highly structure‐sensitive. In this way, we also demonstrate how the simultaneous collection of spectroscopic and kinetic data during modulated or transient experiments is a powerful tool for investigating solid catalysts under realistic operation conditions. [ABSTRACT FROM AUTHOR] – Name: AbstractSuppliedCopyright Label: Group: Ab Data: <i>Copyright of ChemCatChem is the property of Wiley-Blackwell and its content may not be copied or emailed to multiple sites without the copyright holder's express written permission. Additionally, content may not be used with any artificial intelligence tools or machine learning technologies. However, users may print, download, or email articles for individual use. This abstract may be abridged. No warranty is given about the accuracy of the copy. Users should refer to the original published version of the material for the full abstract.</i> (Copyright applies to all Abstracts.) |
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| RecordInfo | BibRecord: BibEntity: Identifiers: – Type: doi Value: 10.1002/cctc.202301447 Languages: – Code: eng Text: English PhysicalDescription: Pagination: PageCount: 9 StartPage: 1 Subjects: – SubjectFull: Modulation spectroscopy Type: general – SubjectFull: Fourier transform infrared spectroscopy Type: general – SubjectFull: Catalysts Type: general – SubjectFull: Catalyst supports Type: general – SubjectFull: Catalytic activity Type: general Titles: – TitleFull: Probing the Reactive Intermediates in CO2 Hydrogenation on Ni/Al2O3 Catalysts with Modulation Excitation Spectroscopy. Type: main BibRelationships: HasContributorRelationships: – PersonEntity: Name: NameFull: Kock, Mikkel – PersonEntity: Name: NameFull: Kowalewski, Emil – PersonEntity: Name: NameFull: Iltsiou, Dimitra – PersonEntity: Name: NameFull: Mielby, Jerrik – PersonEntity: Name: NameFull: Kegnæs, Søren IsPartOfRelationships: – BibEntity: Dates: – D: 22 M: 02 Text: 2/22/2024 Type: published Y: 2024 Identifiers: – Type: issn-print Value: 18673880 Numbering: – Type: volume Value: 16 – Type: issue Value: 4 Titles: – TitleFull: ChemCatChem Type: main |
| ResultId | 1 |
