CO2 Methanation over Rh/CeO2 Studied with Infrared Modulation Excitation Spectroscopy and Phase Sensitive Detection
Journal article, 2020

Methane is a well-established fuel molecule whose production from CO2 through methanation garners increasing interest as an energy storage solution. While often produced with Ni based catalysts, other metals are of interest thanks to higher robustness and activity-selectivity numbers. The Rh/CeO2 catalyst has shown appreciable properties for CO2 methanation and its structural dynamics has been studied in situ. However, the reaction pathway is unknown. Here, we present infrared modulation excitation spectroscopy measurements with phase sensitive detection of a Rh/CeO2 catalyst adsorbate composition during H2 pulsing (0–2 vol.%) to a constant CO2 (0.5 vol.%) feed. Various carbonyl (CO) and carbonate (b-CO3 /p-CO3 ) ad-species clearly respond to the hydrogen stimulus, making them potential reaction intermediates. The different CO ad-species are likely intermediates for product CO and CH4 but their individual contributions to the respective formations are not unambiguously ascertained. As for the carbonate dynamics, it might be linked to the reduction/oxidation of the CeO2 surface upon H2 pulsing. Formate (HCOO) ad-species are clearly visible but appear to be, if not spectators, linked to slow side reactions possibly also affected by CeO2 redox processes.

carbon cycling

phase sensitive detection

modulation excitation spectroscopy

surface intermediates

catalytic mechanisms

supported catalyst

hydrogenation

diffuse reflectance

CO2 utilisation

Author

Felix Hemmingsson

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

Andreas Schaefer

Chalmers, Chemistry and Chemical Engineering, Applied Chemistry

Magnus Skoglundh

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

Per-Anders Carlsson

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

Catalysts

2073-4344 (ISSN)

Vol. 10 6 601

Atomistic Design of Catalysts

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

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

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

Subject Categories

Inorganic Chemistry

Other Chemical Engineering

Driving Forces

Sustainable development

Areas of Advance

Energy

Materials Science

Roots

Basic sciences

DOI

10.3390/catal10060601

More information

Latest update

10/22/2020