Ouyang, M;
Papanikolaou, KG;
Boubnov, A;
Hoffman, AS;
Giannakakis, G;
Bare, SR;
Stamatakis, M;
... Sykes, ECH; + view all
(2021)
Directing reaction pathways via in situ control of active site geometries in PdAu single-atom alloy catalysts.
Nature Communications
, 12
, Article 1549. 10.1038/s41467-021-21555-z.
Preview |
Text
Stamatakis_s41467-021-21555-z.pdf - Published Version Download (4MB) | Preview |
Abstract
The atomic scale structure of the active sites in heterogeneous catalysts is central to their reactivity and selectivity. Therefore, understanding active site stability and evolution under different reaction conditions is key to the design of efficient and robust catalysts. Herein we describe theoretical calculations which predict that carbon monoxide can be used to stabilize different active site geometries in bimetallic alloys and then demonstrate experimentally that the same PdAu bimetallic catalyst can be transitioned between a single-atom alloy and a Pd cluster phase. Each state of the catalyst exhibits distinct selectivity for the dehydrogenation of ethanol reaction with the single-atom alloy phase exhibiting high selectivity to acetaldehyde and hydrogen versus a range of products from Pd clusters. First-principles based Monte Carlo calculations explain the origin of this active site ensemble size tuning effect, and this work serves as a demonstration of what should be a general phenomenon that enables in situ control over catalyst selectivity.
| Type: | Article |
|---|---|
| Title: | Directing reaction pathways via in situ control of active site geometries in PdAu single-atom alloy catalysts |
| Open access status: | An open access version is available from UCL Discovery |
| DOI: | 10.1038/s41467-021-21555-z |
| Publisher version: | https://doi.org/10.1038/s41467-021-21555-z |
| Language: | English |
| Additional information: | s This article is licensed under a Creative Commons Attribution 4.0 International License, which permits use, sharing, adaptation, distribution and reproduction in any medium or format, as long as you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons license, and indicate if changes were made. The images or other third party material in this article are included in the article’s Creative Commons license, unless indicated otherwise in a credit line to the material. If material is not included in the article’s Creative Commons license and your intended use is not permitted by statutory regulation or exceeds the permitted use, you will need to obtain permission directly from the copyright holder. To view a copy of this license, visit http://creativecommons.org/ licenses/by/4.0/. |
| UCL classification: | UCL UCL > Provost and Vice Provost Offices > UCL BEAMS 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 |
| URI: | https://discovery.ucl.ac.uk/id/eprint/10123707 |
Archive Staff Only
 |
View Item |
