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

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Názov: Structure-function relationship for CO2 methanation over ceria supported Rh and Ni catalysts under atmospheric pressure conditions
Autori: Martin, Natalia Mihaela, 1984, Hemmingsson, Felix, 1992, Schaefer, Andreas, 1981, Ek, Martin, Merte, L. R., Hejral, Uta, 1984, Gustafsson, Johan, Skoglundh, Magnus, 1965, Dippel, Ann Christin, Gutowski, Olof, Bauer, Matthias, Carlsson, Per-Anders, 1972
Zdroj: Atomär design av katalysatorer Tidsupplösta in situ metoder för design av katalytiska säten för hållbar kemi Synergistisk utveckling av rötngentekniker och tillämpbara tunna oxider för hållbar kemi Catalysis Science and Technology. 9(7):1644-1653
Popis: 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.
Popis súboru: electronic
Prístupová URL adresa: https://research.chalmers.se/publication/509311
https://research.chalmers.se/publication/509745
https://research.chalmers.se/publication/509745/file/509745_Fulltext.pdf
Databáza: SwePub
Popis
Abstrakt: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.
ISSN:20444753
20444761
DOI:10.1039/C8CY02097C