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 (31) pp. 7314-7319. 10.1021/acs.jpclett.2c01519.

Preview

Text Reocreux_Stick or Spill_AOP.pdf Download (1MB) | Preview

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.

Download activity - last month

Export as XMLJSONCSV

Download activity - last 12 months

Export as JSONCSVXML

Downloads by country - last 12 months

Export as XMLCSVJSON

Archive Staff Only

View Item