The Hydrogenation of Crotonaldehyde on PdCu Single Atom Alloy Catalysts


Recyclable PdCu single atom alloys supported on Al2O3 were applied to the selective hydrogenation of crotonaldehyde to elucidate the minimum number of Pd atoms required to facilitate the sustainable transformation of an α,β-unsaturated carbonyl molecule. It was found that, by diluting the Pd content of the alloy, the reaction activity of Cu nanoparticles can be accelerated, enabling more time for the cascade conversion of butanal to butanol. In addition, a significant increase in the conversion rate was observed, compared to bulk Cu/Al2O3 and Pd/Al2O3 catalysts when normalising for Cu and Pd content, respectively. The reaction selectivity over the single atom alloy catalysts was found to be primarily controlled by the Cu host surface, mainly leading to the formation of butanal but at a significantly higher rate than the monometallic Cu catalyst. Low quantities of crotyl alcohol were observed over all Cu-based catalysts but not for the Pd monometallic catalyst, suggesting that it may be a transient species converted immediately to butanol and or isomerized to butanal. These results demonstrate that fine-tuning the dilution of PdCu single atom alloy catalysts can leverage the activity and selectivity enhancement, and lead to cost-effective, sustainable, and atom-efficient alternatives to monometallic catalysts.

Publication DOI:
Divisions: College of Engineering & Physical Sciences > School of Infrastructure and Sustainable Engineering > Chemical Engineering & Applied Chemistry
College of Engineering & Physical Sciences
College of Engineering & Physical Sciences > Energy and Bioproducts Research Institute (EBRI)
Additional Information: Copyright © 2023 by the authors. Licensee MDPI, Basel, Switzerland. This article is an open access article distributed under the terms and conditions of the Creative Commons Attribution (CC BY) license ( Funding Information & Acknowledgments: G.K. acknowledges funding from EPSRC (EP/M005186/2). M.J.I. acknowledges the award of a PhD scholarship from Aston University. The authors wish to acknowledge the Diamond Light Source and the UK Catalysis Hub for provision of beamtime (proposal number SP19850-6). The authors also acknowledge the Energy Research Accelerator (ERA) for the funding of equipment used in this work.
Uncontrolled Keywords: PdCu,crotonaldehyde,hydrogenation,single atom alloy,single atom catalysts,Chemical Engineering(all),Materials Science(all)
Publication ISSN: 2079-4991
Full Text Link:
Related URLs: https://www.mdp ... -4991/13/8/1434 (Publisher URL)
http://www.scop ... tnerID=8YFLogxK (Scopus URL)
PURE Output Type: Article
Published Date: 2023-04-21
Published Online Date: 2023-04-21
Accepted Date: 2023-04-18
Authors: Islam, Mohammed J.
Granollers Mesa, Marta (ORCID Profile 0000-0001-8602-9362)
Osatiashtiani, Amin (ORCID Profile 0000-0003-1334-127X)
Taylor, Martin J.
Isaacs, Mark A.
Kyriakou, Georgios



Version: Published Version

License: Creative Commons Attribution

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