Lozano-Reis, Pablo;
Prats, Hector;
Sayós, Ramón;
Rodriguez, José A;
Illas, Francesc;
(2021)
Assessing the Activity of Ni Clusters Supported on TiC(001) toward CO2 and H2 Dissociation.
The Journal of Physical Chemistry C
, 125
(22)
pp. 12019-12027.
10.1021/acs.jpcc.1c03219.
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Abstract
Small Ni particles supported on TiC(001) were shown to display a very high activity for the catalytic hydrogenation of CO2but the underlying chemistry is, to a large extent, unknown. Here, by means of periodic density functional theory (DFT) calculations with the BEEF-vdW functional, we explore the adsorption and subsequent dissociation of CO2and H2on several Ninclusters (n= 4, 9, 13, and 16) supported on TiC(001) and compare the results to those obtained for the bare Ni(111) and TiC(001) surfaces using exactly the same computational approach. The calculations reveal that the Nin/TiC system exhibits stronger adsorption energies and lower dissociation energy barriers for CO2and H2than the bare Ni(111) and TiC(001) surfaces. This is in line with the experimental finding evidencing that the Ni/TiC system has a catalytic activity higher than that of the separated Ni and TiC constituents. In addition, the calculated results show that two-dimensional (2D) supported clusters adsorb CO2and H2stronger than the three-dimensional (3D) supported clusters and also the 2D clusters exhibit lower energy barriers for CO2dissociation. Within the 2D supported clusters, larger particles feature slightly stronger adsorption energies and lower CO2dissociation energy barriers. Finally, H2dissociation proceeds with a very low energy barrier on all of the studied models, which makes these novel systems potential good candidates for hydrogenation reactions.
| Type: | Article |
|---|---|
| Title: | Assessing the Activity of Ni Clusters Supported on TiC(001) toward CO2 and H2 Dissociation |
| Open access status: | An open access version is available from UCL Discovery |
| DOI: | 10.1021/acs.jpcc.1c03219 |
| Publisher version: | https://doi.org/10.1021/acs.jpcc.1c03219 |
| 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: | Science & Technology, Physical Sciences, Technology, Chemistry, Physical, Nanoscience & Nanotechnology, Materials Science, Multidisciplinary, Chemistry, Science & Technology - Other Topics, Materials Science, GENERALIZED GRADIENT APPROXIMATION, GAS SHIFT REACTION, HYDROGENATION REACTIONS, RENEWABLE ENERGY, NOBLE-METALS, CATALYSTS, ACTIVATION, WATER, TRANSITION, ADSORPTION |
| UCL classification: | UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Engineering Science UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Engineering Science > Dept of Chemical Engineering UCL > Provost and Vice Provost Offices > UCL BEAMS UCL |
| URI: | https://discovery.ucl.ac.uk/id/eprint/10155760 |
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