A Multitechnique Study of C 2 H 4 Adsorption on a Model Single-Atom Rh 1 Catalyst.

Autor: Wang C; Institute of Applied Physics, TU Wien, Vienna 1040, Austria., Sombut P; Institute of Applied Physics, TU Wien, Vienna 1040, Austria., Puntscher L; Institute of Applied Physics, TU Wien, Vienna 1040, Austria., Ulreich M; Institute of Applied Physics, TU Wien, Vienna 1040, Austria., Pavelec J; Institute of Applied Physics, TU Wien, Vienna 1040, Austria., Rath D; Institute of Applied Physics, TU Wien, Vienna 1040, Austria., Balajka J; Institute of Applied Physics, TU Wien, Vienna 1040, Austria., Meier M; Institute of Applied Physics, TU Wien, Vienna 1040, Austria.; Faculty of Physics, Center for Computational Materials Science, University of Vienna, Vienna 1090, Austria., Schmid M; Institute of Applied Physics, TU Wien, Vienna 1040, Austria., Diebold U; Institute of Applied Physics, TU Wien, Vienna 1040, Austria., Franchini C; Faculty of Physics, Center for Computational Materials Science, University of Vienna, Vienna 1090, Austria.; Dipartimento di Fisica e Astronomia, Università di Bologna, 40126 Bologna ,Italy., Parkinson GS; Institute of Applied Physics, TU Wien, Vienna 1040, Austria.
Jazyk: angličtina
Zdroj: The journal of physical chemistry. C, Nanomaterials and interfaces [J Phys Chem C Nanomater Interfaces] 2024 Sep 05; Vol. 128 (37), pp. 15404-15411. Date of Electronic Publication: 2024 Sep 05 (Print Publication: 2024).
DOI: 10.1021/acs.jpcc.4c03588
Abstrakt: Single-atom catalysts are potentially ideal model systems to investigate structure-function relationships in catalysis if the active sites can be uniquely determined. In this work, we study the interaction of C 2 H 4 with a model Rh/Fe 3 O 4 (001) catalyst that features 2-, 5-, and 6-fold coordinated Rh adatoms, as well as Rh clusters. Using multiple surface-sensitive techniques in combination with calculations of density functional theory (DFT), we follow the thermal evolution of the system and disentangle the behavior of the different species. C 2 H 4 adsorption is strongest at the 2-fold coordinated Rh 1 with a DFT-determined adsorption energy of -2.26 eV. However, desorption occurs at lower temperatures than expected because the Rh migrates into substitutional sites within the support, where the molecule is more weakly bound. The adsorption energy at the 5-fold coordinated Rh sites is predicated to be -1.49 eV, but the superposition of this signal with that from small Rh clusters and additional heterogeneity leads to a broad C 2 H 4 desorption shoulder in TPD above room temperature.
Competing Interests: The authors declare no competing financial interest.
(© 2024 The Authors. Published by American Chemical Society.)
Databáze: MEDLINE
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