Structure–function relationship for CO2 methanation over ceria supported Rh and Ni catalysts under atmospheric pressure conditions

Natalia M. Martin; Felix Hemmingsson; Andreas Schaefer; Martin Ek; Lindsay R. Merte; Uta Hejral; Johan Gustafson; Magnus Skoglundh; Ann-Christin Dippel; Olof Gutowski; Matthias Bauer; Per-Anders Carlsson

doi:10.1039/C8CY02097C

Structure–function relationship for CO₂ methanation over ceria supported Rh and Ni catalysts under atmospheric pressure conditions

Natalia M. Martin,

*^a Felix Hemmingsson,

^a Andreas Schaefer,

^a Martin Ek,

^b Lindsay R. Merte,^c Uta Hejral,^d Johan Gustafson,^d Magnus Skoglundh,

^a Ann-Christin Dippel,

^e Olof Gutowski,^e Matthias Bauer^f and Per-Anders Carlsson

^a

Author affiliations

* Corresponding authors

^a Department of Chemistry and Chemical Engineering and Competence Centre for Catalysis, Chalmers University of Technology, Göteborg, Sweden
E-mail: Natalia.Martin@chalmers.se
Fax: +46 31160062
Tel: +46 31 772 29 04

^b Centre for Analysis and Synthesis, Lund University, 22100 Lund, Sweden

^c Department of Materials Science and Applied Mathematics, Malmö University, 204 06 Malmö, Sweden

^d Division of Synchrotron Radiation Research, Lund University, 22100 Lund, Sweden

^e Deutsches Elektronen-Synchrotron DESY, 22607 Hamburg, Germany

^f Department of Chemistry, Paderborn University, 33098 Paderborn, Germany

Abstract

In situ structural and chemical state characterization of Rh/CeO₂ and Ni/CeO₂ catalysts during atmospheric pressure CO₂ methanation has been performed by a combined array of time-resolved analytical techniques including ambient-pressure X-ray photoelectron spectroscopy, high-energy X-ray diffraction and diffuse reflectance infrared Fourier transform spectroscopy. The ceria phase is partially reduced during the CO₂ methanation and in particular Ce³⁺ species seem to facilitate activation of CO₂ molecules. The activated CO₂ molecules then react with atomic hydrogen provided from H₂ dissociation on Rh and Ni sites to form formate species. For the most active catalyst (Rh/CeO₂), transmission electron microscopy measurements show that the Rh nanoparticles are small (average 4 nm, but with a long tail towards smaller particles) due to a strong interaction between Rh particles and the ceria phase. In contrast, larger nanoparticles were observed for the Ni/CeO₂ catalyst (average 6 nm, with no crystallites below 5 nm found), suggesting a weaker interaction with the ceria phase. The higher selectivity towards methane of Rh/CeO₂ is proposed to be due to the stronger metal–support interaction.

This article is part of the themed collection: 2019 Catalysis Science & Technology HOT Articles

Catalysis Science & Technology

Structure–function relationship for CO₂ methanation over ceria supported Rh and Ni catalysts under atmospheric pressure conditions

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Structure–function relationship for CO₂ methanation over ceria supported Rh and Ni catalysts under atmospheric pressure conditions

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