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Stick or Spill? Scaling Relationships for the Binding Energies of Adsorbates on Single-Atom Alloy Catalysts

Réocreux, Romain; Sykes, E Charles H; Michaelides, Angelos; Stamatakis, Michail; (2022) Stick or Spill? Scaling Relationships for the Binding Energies of Adsorbates on Single-Atom Alloy Catalysts. Journal of Physical Chemistry Letters , 13 pp. 7314-7319. 10.1021/acs.jpclett.2c01519. (In press). Green open access

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Abstract

Single-atom alloy catalysts combine catalytically active metal atoms, present as dopants, with the selectivity of coinage metal hosts. Determining whether adsorbates stick at the dopant or spill over onto the host is key to understanding catalytic mechanisms on these materials. Despite a growing body of work, simple descriptors for the prediction of spillover energies (SOEs), i.e., the relative stability of an adsorbate on the dopant versus the host site, are not yet available. Using Density Functional Theory (DFT) calculations on a large set of adsorbates, we identify the dopant charge and the SOE of carbon as suitable descriptors. Combining them into a linear surrogate model, we can reproduce DFT-computed SOEs within 0.06 eV mean absolute error. More importantly, our work provides an intuitive theoretical framework, based on the concepts of electrostatic interactions and covalency, that explains SOE trends and can guide the rational design of future single-atom alloy catalysts.

Type: Article
Title: Stick or Spill? Scaling Relationships for the Binding Energies of Adsorbates on Single-Atom Alloy Catalysts
Location: United States
Open access status: An open access version is available from UCL Discovery
DOI: 10.1021/acs.jpclett.2c01519
Publisher version: https://doi.org/10.1021/acs.jpclett.2c01519
Language: English
Additional information: © 2022 The Authors. Published by American Chemical Society under the terms of the Creative Commons Attribution 4.0 International (CC BY 4.0) Licence (https://creativecommons.org/licenses/by/4.0/).
Keywords: Adsorption, Catalysts, Electrostatics, Impurities, Metals
UCL classification: UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Maths and Physical Sciences
UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Maths and Physical Sciences > Dept of Physics and Astronomy
UCL > Provost and Vice Provost Offices > UCL BEAMS
UCL
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/10153553
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