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An ab initio study of size-selected Pd nanocluster catalysts for the hydrogenation of 1-pentyne

Theodoros Pavloudis, Joseph Kioseoglou Orcid Logo, Richard Palmer Orcid Logo

Physical Chemistry Chemical Physics, Volume: 24, Issue: 5, Pages: 3231 - 3237

Swansea University Authors: Theodoros Pavloudis, Richard Palmer Orcid Logo

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DOI (Published version): 10.1039/d1cp05470h

Abstract

The hydrogenation of alkynes is an important reaction in the synthesis of both fine and bulk chemicals. Palladium-based catalysts are widely used and therefore size-selected Pd nanoclusters may provide enhanced performance. An investigation of the adsorption and desorption of the molecules involved...

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Published in: Physical Chemistry Chemical Physics
ISSN: 1463-9076 1463-9084
Published: Royal Society of Chemistry (RSC) 2022
Online Access: Check full text

URI: https://cronfa.swan.ac.uk/Record/cronfa59203
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Abstract: The hydrogenation of alkynes is an important reaction in the synthesis of both fine and bulk chemicals. Palladium-based catalysts are widely used and therefore size-selected Pd nanoclusters may provide enhanced performance. An investigation of the adsorption and desorption of the molecules involved in the reaction can shed light on the activity and selectivity of the catalysts. We employ ab initio calculations to investigate the binding energies of all the molecules related to the hydrogenation of 1-pentyne (1-pentyne, 1-pentene, cis-2-pentene, trans-2-pentene and pentane) on a comprehensive set of possible binding sites of two Pd147 and Pd561 cuboctahedral nanoclusters. We extract the site and size dependence of these binding energies. We find that the adsorption of 1-pentyne occurs preferably on the (100) facets of the nanoclusters, followed by their (111) facets, their edges and their vertices. The molecule binds more strongly on the larger nanoclusters, which are therefore expected to display higher activity. The binding energies of the pentenes are found to be lower on the smaller nanoclusters. Therefore, these molecules are expected to desorb more easily and the small clusters should display better selectivity, i.e., partial hydrogenation to 1-pentene, compared with large clusters. Our results provide guidelines for the optimal design of Pd nanocatalysts.
College: College of Engineering
Funders: This work was financially supported by the Engineering and Physical Sciences Research Council
Issue: 5
Start Page: 3231
End Page: 3237