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Catalytic Reduction of Carbon Dioxide on the (001), (011), and (111) Surfaces of TiC and ZrC: A Computational Study

Silveri, Fabrizio; Quesne, Matthew G; Viñes, Francesc; Illas, Francesc; Catlow, C Richard A; de Leeuw, Nora H; (2022) Catalytic Reduction of Carbon Dioxide on the (001), (011), and (111) Surfaces of TiC and ZrC: A Computational Study. The Journal of Physical Chemistry C , 126 (11) pp. 5138-5150. 10.1021/acs.jpcc.1c10180. Green open access

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Abstract

We present a computational study of the activity and selectivity of early transition-metal carbides as carbon dioxide reduction catalysts. We analyze the effects of the adsorption of CO_{2} and H_{2} on the (001), (011), and metal-terminated (111) surfaces of TiC and ZrC, as carbon dioxide undergoes either dissociation to CO or hydrogenation to COOH or HCOO. The relative stabilities of the three reduction intermediates and the activation energies for their formation allow the identification of favored pathways on each surface, which are examined as they lead to the release of CO, HCOOH, CH_{3}OH, and CH_{4}, thereby also characterizing the activity and selectivity of the two materials. Reaction energetics implicate HCO as the key common intermediate on all surfaces studied and rule out the release of formaldehyde. Surface hydroxylation is shown to be highly selective toward methane production as the formation of methanol is hindered on all surfaces by its barrierless conversion to CO.

Type: Article
Title: Catalytic Reduction of Carbon Dioxide on the (001), (011), and (111) Surfaces of TiC and ZrC: A Computational Study
Open access status: An open access version is available from UCL Discovery
DOI: 10.1021/acs.jpcc.1c10180
Publisher version: https://doi.org/10.1021/acs.jpcc.1c10180
Language: English
Additional information: © The Author 2022. Original content in this article is licensed under the terms of the Creative Commons Attribution 4.0 International (CC BY 4.0) Licence (https://creativecommons.org/licenses/by/4.0/).
UCL classification: 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
UCL > Provost and Vice Provost Offices > UCL BEAMS
UCL
URI: https://discovery.ucl.ac.uk/id/eprint/10145641
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