Alonso, Gerard;
López, Estefanía;
Huarte-Larrañaga, Fermín;
Sayós, Ramón;
Prats, Hector;
Gamallo, Pablo;
(2021)
Zeolite-encapsulated single-atom catalysts for efficient CO2 conversion.
Journal of CO2 Utilization
, 54
, Article 101777. 10.1016/j.jcou.2021.101777.
Preview |
Text
1-s2.0-S2212982021003449-main.pdf - Published Version Download (5MB) | Preview |
Abstract
Zeolite-supported single-atom catalysts (SACs) have emerged as a novel class of cheap and tuneable catalysts that can exhibit high activity, selectivity and stability. In this work, we conduct an extensive screening by means of density functional theory calculations to determine the usefulness of 3d, 4d and 5d transition metal (TM) SACs-supported in MFI-type Silicalite-1 zeolite for CO2 conversion. Two reaction mechanisms are considered, namely the redox direct CO2 dissociation and associative hydrogen-assisted CO2 dissociation mechanisms. Early TM SACs exhibit the lowest energy barriers, which follow the redox mechanism. These energy barriers raise when going right in the periodic table up to group 10, where they become prohibitive and the associative mechanism should dominate. By also considering their resistance to aggregation, we support the use of Sc, Y, La, Ru, Rh, Ni, Pd and Pt as potentially active and stable catalysts for CO2 conversion, given their low energy barriers and strong interaction with the zeolite framework.
| Type: | Article |
|---|---|
| Title: | Zeolite-encapsulated single-atom catalysts for efficient CO2 conversion |
| Open access status: | An open access version is available from UCL Discovery |
| DOI: | 10.1016/j.jcou.2021.101777 |
| Publisher version: | https://doi.org/10.1016/j.jcou.2021.101777 |
| Language: | English |
| Additional information: | © 2021 The Author(s). Published by Elsevier Ltd. This is an open access article under the CC BY license (http://creativecommons.org/licenses/by/4.0/). |
| Keywords: | Single-atom catalysts, Zeolites, MFI, Heterogeneous catalysis, CO2 conversion, Transition metals, Density functional theory |
| 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/10153205 |
Loading...
Loading...Loading...Loading...Archive Staff Only
 |
View Item |
