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The Effect of CO Partial Pressure on Important Kinetic Parameters of Methanation Reaction on Co-Based FTS Catalyst Studied by SSITKA-MS and Operando DRIFTS-MS Techniques
Open AccessArticle

CO2 Methanation over Rh/CeO2 Studied with Infrared Modulation Excitation Spectroscopy and Phase Sensitive Detection

Department of Chemistry and Chemical Engineering and Competence Centre for Catalysis, Chalmers University of Technology, 412 96 Gothenburg, Sweden
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Catalysts 2020, 10(6), 601; https://doi.org/10.3390/catal10060601
Received: 11 May 2020 / Revised: 25 May 2020 / Accepted: 26 May 2020 / Published: 29 May 2020
(This article belongs to the Special Issue In Situ and Operando Vibrational Spectroscopy in Catalysis)
Methane is a well-established fuel molecule whose production from CO 2 through methanation garners increasing interest as an energy storage solution. While often produced with Ni based catalysts, other metals are of interest thanks to higher robustness and activity-selectivity numbers. The Rh/CeO 2 catalyst has shown appreciable properties for CO 2 methanation and its structural dynamics has been studied in situ. However, the reaction pathway is unknown. Here, we present infrared modulation excitation spectroscopy measurements with phase sensitive detection of a Rh/CeO 2 catalyst adsorbate composition during H 2 pulsing (0–2 vol.%) to a constant CO 2 (0.5 vol.%) feed. Various carbonyl (CO) and carbonate (b-CO 3 /p-CO 3 ) ad-species clearly respond to the hydrogen stimulus, making them potential reaction intermediates. The different CO ad-species are likely intermediates for product CO and CH 4 but their individual contributions to the respective formations are not unambiguously ascertained. As for the carbonate dynamics, it might be linked to the reduction/oxidation of the CeO 2 surface upon H 2 pulsing. Formate (HCOO) ad-species are clearly visible but appear to be, if not spectators, linked to slow side reactions possibly also affected by CeO 2 redox processes. View Full-Text
Keywords: carbon cycling; CO2 utilisation; hydrogenation; supported catalyst; surface intermediates; catalytic mechanisms; diffuse reflectance; modulation excitation spectroscopy; phase sensitive detection carbon cycling; CO2 utilisation; hydrogenation; supported catalyst; surface intermediates; catalytic mechanisms; diffuse reflectance; modulation excitation spectroscopy; phase sensitive detection
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MDPI and ACS Style

Hemmingsson, F.; Schaefer, A.; Skoglundh, M.; Carlsson, P.-A. CO2 Methanation over Rh/CeO2 Studied with Infrared Modulation Excitation Spectroscopy and Phase Sensitive Detection. Catalysts 2020, 10, 601.

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