UCL Discovery
UCL home » Library Services » Electronic resources » UCL Discovery

Directing reaction pathways via in situ control of active site geometries in PdAu single-atom alloy catalysts

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. Green open access

[thumbnail of Stamatakis_s41467-021-21555-z.pdf]
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
Downloads since deposit
17Downloads
Download activity - last month
Download activity - last 12 months
Downloads by country - last 12 months

Archive Staff Only

View Item View Item