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

Published version
Peer-reviewed

Type

Article

Change log

Authors

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.

Description

Keywords

51 Physical Sciences, 34 Chemical Sciences, 3406 Physical Chemistry

Journal Title

J Phys Chem Lett

Conference Name

Journal ISSN

1948-7185
1948-7185

Volume Title

13

Publisher

American Chemical Society (ACS)
Sponsorship
Basic Energy Sciences (DE-SC0004738)
Engineering and Physical Sciences Research Council (EP/T022213/1, EP/P020194/1)
Leverhulme Trust (RPG-2018-209)