Periodic Trends in Adsorption Energies around Single-Atom Alloy Active Sites

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Periodic Trends in Adsorption Energies around Single-Atom Alloy Active Sites

Schumann, J; Bao, Y; Hannagan, RT; Sykes, ECH; Stamatakis, M; Michaelides, A; (2021) Periodic Trends in Adsorption Energies around Single-Atom Alloy Active Sites. Journal of Physical Chemistry Letters , 12 pp. 10060-10067. 10.1021/acs.jpclett.1c02497. Green open access

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Abstract

Single-atom alloys (SAAs) make up a special class of alloy surface catalysts that offer well-defined, isolated active sites in a more inert metal host. The dopant sites are generally assumed to have little or no influence on the properties of the host metal, and transport of chemical reactants and products to and from the dopant sites is generally assumed to be facile. Here, by performing density functional theory calculations and surface science experiments, we identify a new physical effect on SAA surfaces, whereby adsorption is destabilized by ≤300 meV on host sites within the perimeter of the reactive dopant site. We identify periodic trends for this behavior and demonstrate a zone of exclusion around the reactive sites for a range of adsorbates and combinations of host and dopant metals. Experiments confirm an increased barrier for diffusion of CO toward the dopant on a RhCu SAA. This effect offers new possibilities for understanding and designing active sites with tunable energetic landscapes surrounding them.

Type:	Article
Title:	Periodic Trends in Adsorption Energies around Single-Atom Alloy Active Sites
Location:	United States
Open access status:	An open access version is available from UCL Discovery
DOI:	10.1021/acs.jpclett.1c02497
Publisher version:	https://doi.org/10.1021/acs.jpclett.1c02497
Language:	English
Additional information:	This version is the author accepted manuscript. For information on re-use, please refer to the publisher’s terms and conditions.
UCL classification:	UCL UCL > Provost and Vice Provost Offices > UCL BEAMS 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 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
URI:	https://discovery.ucl.ac.uk/id/eprint/10136514