Structure-function relationship during CO2 methanation over ceria supported Rh and Ni catalysts at atmospheric pressure conditions
Journal article, 2019

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 CO2methanation 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.

Author

Natalia Mihaela Martin

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

Competence Centre for Catalysis (KCK)

Felix Hemmingsson

Competence Centre for Catalysis (KCK)

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

Andreas Schaefer

Chalmers, Chemistry and Chemical Engineering, Applied Chemistry

Martin Ek Rosén

Lund University

Lindsay R. Merte

Malmö university

Uta Hejral

Lund University

Johan Gustafson

Lund University

Magnus Skoglundh

Chalmers, Chemistry and Chemical Engineering, Applied Chemistry

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

Catalysis Science and Technology

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

Vol. 9 1644-1653

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.

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

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

Driving Forces

Sustainable development

Areas of Advance

Nanoscience and Nanotechnology (2010-2017)

Energy

Materials Science

Subject Categories

Chemical Process Engineering

Other Environmental Engineering

Materials Chemistry

Condensed Matter Physics

DOI

10.1039/C8CY02097C

More information

Latest update

4/2/2019 6