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. ORCID: https://orcid.org/0000-0002-1341-1541 and de Leeuw, Nora H. ORCID: https://orcid.org/0000-0002-8271-0545 2022. Catalytic reduction of carbon dioxide on the (001), (011), and (111) surfaces of TiC and ZrC: a computational study. Journal of Physical Chemistry C 126 (11) , 5138–5150. 10.1021/acs.jpcc.1c10180

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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 CO2 and H2 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, CH3OH, and CH4, 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.

Item Type:	Article
Date Type:	Publication
Status:	Published
Schools:	Advanced Research Computing @ Cardiff (ARCCA) Cardiff Catalysis Institute (CCI) Chemistry
Publisher:	American Chemical Society
ISSN:	1932-7447
Funders:	EPSRC
Date of First Compliant Deposit:	28 March 2022
Date of Acceptance:	16 February 2022
Last Modified:	02 Aug 2024 09:13
URI:	https://orca.cardiff.ac.uk/id/eprint/148925

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