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- Title
Probing the Reactive Intermediates in CO<sub>2</sub> Hydrogenation on Ni/Al<sub>2</sub>O<sub>3</sub> Catalysts with Modulation Excitation Spectroscopy.
- Authors
Kock, Mikkel; Kowalewski, Emil; Iltsiou, Dimitra; Mielby, Jerrik; Kegnæs, Søren
- 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.
- Subjects
MODULATION spectroscopy; FOURIER transform infrared spectroscopy; CATALYSTS; CATALYST supports; CATALYTIC activity
- Publication
ChemCatChem, 2024, Vol 16, Issue 4, p1
- ISSN
1867-3880
- Publication type
Article
- DOI
10.1002/cctc.202301447