Digging Its Own Site
- Author(s)
- Ali Rafsanjani-Abbasi, Florian Buchner, Faith J. Lewis, Lena Puntscher, Florian Kraushofer, Panukorn Sombut, Moritz Eder, Jiří Pavelec, Erik Rheinfrank, Giada Franceschi, Viktor Birschitzky, Michele Riva, Cesare Franchini, Michael Schmid, Ulrike Diebold, Matthias Meier, Georg K.H. Madsen, Gareth S. Parkinson
- Abstract
Determining the local coordination of the active site is a prerequisite for the reliable modeling of single-atom catalysts (SACs). Obtaining such information is difficult on powder-based systems and much emphasis is placed on density functional theory computations based on idealized low-index surfaces of the support. In this work, we investigate how Pt atoms bind to the (11̅02) facet of α-Fe2O3; a common support material in SACs. Using a combination of scanning tunneling microscopy, X-ray photoelectron spectroscopy, and an extensive computational evolutionary search, we find that Pt atoms significantly reconfigure the support lattice to facilitate a pseudolinear coordination to surface oxygen atoms. Despite breaking three surface Fe-O bonds, this geometry is favored by 0.84 eV over the best configuration involving an unperturbed support. We suggest that the linear O-Pt-O configuration is common in reactive Pt-based SAC systems because it balances thermal stability with the ability to adsorb reactants from the gas phase. Moreover, we conclude that extensive structural searches are necessary to determine realistic active site geometries in single-atom catalysis.
- Organisation(s)
- Computational Materials Physics
- External organisation(s)
- Technische Universität Wien, University of Bologna
- Journal
- ACS Nano
- Volume
- 18
- Pages
- 26920-26927
- No. of pages
- 8
- ISSN
- 1936-0851
- DOI
- https://doi.org/10.1021/acsnano.4c08781
- Publication date
- 10-2024
- Peer reviewed
- Yes
- Austrian Fields of Science 2012
- 103018 Materials physics
- Keywords
- ASJC Scopus subject areas
- General Materials Science, General Engineering, General Physics and Astronomy
- Portal url
- https://ucrisportal.univie.ac.at/en/publications/b71bf6cd-07d7-429d-91eb-2bc055b544f4