The Hydrogenation of Crotonaldehyde on PdCu Single Atom Alloy Catalysts

Author:

Islam Mohammed J.1ORCID,Granollers Mesa Marta1,Osatiashtiani Amin1ORCID,Taylor Martin J.2ORCID,Isaacs Mark A.34ORCID,Kyriakou Georgios15ORCID

Affiliation:

1. Energy & Bioproducts Research Institute (EBRI), College of Engineering and Physical Sciences, Aston University, Aston Triangle, Birmingham B4 7ET, UK

2. School of Engineering, Chemical Engineering, University of Hull, Cottingham Road, Hull HU6 7RX, UK

3. Department of Chemistry, University College London, London WC1H 0AJ, UK

4. HarwellXPS, Research Complex at Harwell, Rutherford Appleton Laboratory, Didcot OX11 0FA, UK

5. Department of Chemical Engineering, University of Patras, Caratheodory 1, 265 04 Patras, Greece

Abstract

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.

Funder

Engineering and Physical Sciences Research Council

Publisher

MDPI AG

Subject

General Materials Science,General Chemical Engineering

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