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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.
Original language | English |
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Pages (from-to) | 26920-26927 |
Number of pages | 8 |
Journal | ACS Nano |
Volume | 18 |
Issue number | 39 |
DOIs | |
Publication status | Published - 1 Oct 2024 |
Austrian Fields of Science 2012
- 103018 Materials physics
Keywords
- adsorption site
- hematite
- iron oxide
- platinum
- single-atom catalysis
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Dive into the research topics of 'Digging Its Own Site: Linear Coordination Stabilizes a Pt1/Fe2O3 Single-Atom Catalyst'. Together they form a unique fingerprint.Projects
- 1 Active
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TACO: Taming Complexity in Materials Modeling
Diebold, U., Kresse, G., Mezger-Backus, E. H. G., Dellago, C. & Franchini, C.
1/03/21 → 28/02/29
Project: Research funding