Structure-function relationship for CO2 methanation over ceria supported Rh and Ni catalysts under atmospheric pressure conditions
Artikel i vetenskaplig tidskrift, 2019
In situ structural and chemical state characterization of Rh/CeO 2 and Ni/CeO 2 catalysts during atmospheric pressure CO 2 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 CO 2 methanation and in particular Ce 3+ species seem to facilitate activation of CO 2 molecules. The activated CO 2 molecules then react with atomic hydrogen provided from H 2 dissociation on Rh and Ni sites to form formate species. For the most active catalyst (Rh/CeO 2 ), 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/CeO 2 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/CeO 2 is proposed to be due to the stronger metal-support interaction.
Författare
Natalia Mihaela Martin
Chalmers, Kemi och kemiteknik, Tillämpad kemi
Kompetenscentrum katalys
Felix Hemmingsson
Kompetenscentrum katalys
Chalmers, Kemi och kemiteknik, Tillämpad kemi
Andreas Schaefer
Chalmers, Kemi och kemiteknik, Tillämpad kemi
Kompetenscentrum katalys
Martin Ek
Lunds universitet
L. R. Merte
Malmö universitet
Uta Hejral
Lunds universitet
Johan Gustafsson
Lunds universitet
Magnus Skoglundh
Chalmers, Kemi och kemiteknik, Tillämpad kemi
Ann Christin Dippel
Deutsches Elektronen-Synchrotron (DESY)
Olof Gutowski
Deutsches Elektronen-Synchrotron (DESY)
Matthias Bauer
Universität Paderborn
Per-Anders Carlsson
Chalmers, Kemi och kemiteknik, Tillämpad kemi
Kompetenscentrum katalys
Catalysis Science and Technology
2044-4753 (ISSN) 2044-4761 (eISSN)
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DOI
10.1039/C8CY02097C