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  Isolated Pd atoms in a silver matrix: Spectroscopic and chemical properties

Hartwig, C., Schweinar, K., Jones, T., Beeg, S., Schmidt, F., Schlögl, R., et al. (2021). Isolated Pd atoms in a silver matrix: Spectroscopic and chemical properties. The Journal of Chemical Physics, 154(18): 184703. doi:/10.1063/5.0045936.

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 Creators:
Hartwig, Caroline1, Author
Schweinar, Kevin2, Author
Jones, Travis3, Author              
Beeg, Sebastian1, Author
Schmidt, Franz1, 3, Author              
Schlögl, Robert1, 3, Author              
Greiner, Mark1, Author
Affiliations:
1Max Planck Institute for Chemical Energy Conversion, Mülheim an der Ruhr, Germany, ou_persistent22              
2Max-Planck-Institut für Eisenforschung GmbH , Düsseldorf, Germany, ou_persistent22              
3Inorganic Chemistry, Fritz Haber Institute, Max Planck Society, ou_24023              

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 Abstract: Over the past decade, single-atom alloys (SAAs) have been a lively topic of research due to their potential for achieving novel catalytic properties and circumventing some known limitations of heterogeneous catalysts, such as scaling relationships. In researching SAAs, it is important to recognize experimental evidence of peculiarities in their electronic structure. When an isolated atom is embedded in a matrix of foreign atoms, it exhibits spectroscopic signatures that reflect its surrounding chemical environment. In the present work, using photoemission spectroscopy and computational chemistry, we discuss the experimental evidence from Ag0.98Pd0.02 SAAs that show free-atom-like characteristics in their electronic structure. In particular, the broad Pd4d valence band states of the bulk Pd metal become a narrow band in the alloy. The measured photoemission spectra were compared with the calculated photoemission signal of a free Pd atom in the gas phase with very good agreement, suggesting that the Pd4d states in the alloy exhibit very weak hybridization with their surroundings and are therefore electronically isolated. Since AgPd alloys are known for their superior performance in the industrially relevant semi-hydrogenation of acetylene, we considered whether it is worthwhile to drive the dilution of Pd in the inert Ag host to the single-atom level. We conclude that although site-isolation provides beneficial electronic structure changes to the Pd centers due to the difficulty in activating H2 on Ag, utilizing such SAAs in acetylene semi-hydrogenation would require either a higher Pd concentration to bring isolated sites sufficiently close together or an H2-activating support.

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Language(s): eng - English
 Dates: 2021-01-302021-04-212021-05-112021-05-14
 Publication Status: Published in print
 Pages: 9
 Publishing info: -
 Table of Contents: -
 Rev. Type: Peer
 Identifiers: DOI: /10.1063/5.0045936
 Degree: -

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Title: The Journal of Chemical Physics
  Abbreviation : J. Chem. Phys.
Source Genre: Journal
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Publ. Info: Woodbury, N.Y. : American Institute of Physics
Pages: 9 Volume / Issue: 154 (18) Sequence Number: 184703 Start / End Page: - Identifier: ISSN: 0021-9606
CoNE: https://pure.mpg.de/cone/journals/resource/954922836226