Clark, AH;
Beyer, KA;
Hayama, S;
Hyde, TI;
Sankar, G;
(2019)
The Unusual Redox Behaviour of Ceria and its Interaction with Hydrogen.
Chemistry of Materials
, 31
(18)
pp. 7744-7751.
10.1021/acs.chemmater.9b02854.
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Abstract
The reaction between ceria and hydrogen has been subject to numerous theoretical and experimental studies because of its importance as a catalytic material. Here, we present dynamic and reversible evolution of the cerium oxidation states observed through X-ray absorption spectroscopy experiments in addition to the investigation of associated lattice expansion and contraction through X-ray diffraction and PDF methods. Employing a novel calculation of the temperature dependence of the Gibbs free energy through consideration of the relationship between the instantaneous thermal lattice expansion and the rate of change of the cerium oxidation state, the unusual redox chemistry is reported here. This unusual behavior is interpreted to be due to the formation of a metastable cerium oxyhydride as suggested.
| Type: | Article |
|---|---|
| Title: | The Unusual Redox Behaviour of Ceria and its Interaction with Hydrogen |
| Open access status: | An open access version is available from UCL Discovery |
| DOI: | 10.1021/acs.chemmater.9b02854 |
| Publisher version: | https://doi.org/10.1021/acs.chemmater.9b02854 |
| Language: | English |
| Additional information: | This version is the author accepted manuscript. For information on re-use, please refer to the publisher’s terms and conditions. |
| Keywords: | Redox reactions, Hydrogen, Oxides, Lattices, Oxygen |
| UCL classification: | UCL UCL > Provost and Vice Provost Offices > UCL BEAMS UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Maths and Physical Sciences UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Maths and Physical Sciences > Dept of Chemistry |
| URI: | https://discovery.ucl.ac.uk/id/eprint/10081187 |
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