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

Author

Natalia Mihaela Martin

Chalmers, Chemistry and Chemical Engineering, Applied Chemistry, Per-Anders Carlsson Group

Competence Centre for Catalysis (KCK)

Felix Hemmingsson

Chalmers, Chemistry and Chemical Engineering, Applied Chemistry, Per-Anders Carlsson Group

Competence Centre for Catalysis (KCK)

Andreas Schaefer

Competence Centre for Catalysis (KCK)

Chalmers, Chemistry and Chemical Engineering, Applied Chemistry

Martin Ek

Lund University

L. R. Merte

Malmö university

Uta Hejral

Lund University

Johan Gustafsson

Lund University

Magnus Skoglundh

Chalmers, Chemistry and Chemical Engineering, Applied Chemistry, Polymer Technology

Ann Christin Dippel

Deutsches Elektronen-Synchrotron (DESY)

Olof Gutowski

Deutsches Elektronen-Synchrotron (DESY)

Matthias Bauer

Padernborn University

Per-Anders Carlsson

Chalmers, Chemistry and Chemical Engineering, Applied Chemistry, Per-Anders Carlsson Group

Competence Centre for Catalysis (KCK)

Catalysis Science and Technology

2044-4753 (ISSN) 2044-4761 (eISSN)

Vol. 9 7 1644-1653

Time-resolved in situ methods for design of catalytic sites within sustainable chemistry

Swedish Research Council (VR), 2013-01-01 -- 2016-12-31.

Synergistic development of X-ray techniques and applicable thin oxides for sustainable chemistry

Swedish Research Council (VR), 2018-04-04 -- 2021-12-31.

Atomistic Design of Catalysts

Knut and Alice Wallenberg Foundation, 2016-01-07 -- 2021-06-30.

Driving Forces

Sustainable development

Areas of Advance

Energy

Materials Science

Subject Categories

Materials Chemistry

DOI

10.1039/c8cy02097c

More information

Latest update

6/12/2019