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

Schumann, Julia; Bao, Yutian; Hannagan, Ryan T.; Sykes, E. Charles H.; Stamatakis, Michail; Michaelides, Angelos

doi:10.1021/acs.jpclett.1c02497

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

Journal Article · Mon Oct 11 00:00:00 EDT 2021 · Journal of Physical Chemistry Letters

DOI:https://doi.org/10.1021/acs.jpclett.1c02497· OSTI ID:1844969

^[1]; Bao, Yutian ^[2]; Hannagan, Ryan T. ^[3];

^[3];

^[2];

^[1]

Univ. College London (United Kingdom); Univ. of Cambridge (United Kingdom)
Univ. College London (United Kingdom)
Tufts Univ., Medford, MA (United States)

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. Furthermore, this effect offers new possibilities for understanding and designing active sites with tunable energetic landscapes surrounding them.

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Research Organization:: Tufts Univ., Medford, MA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: SC0004738

OSTI ID:: 1844969

Journal Information:: Journal of Physical Chemistry Letters, Vol. 12, Issue 41; ISSN 1948-7185

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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