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  Interfacial charge distributions in carbon-supported palladium catalysts

Rao, R. G., Blume, R., Hansen, T. W., Fuentes, E., Dreyer, K., Moldovan, S., et al. (2017). Interfacial charge distributions in carbon-supported palladium catalysts. Nature Communications, 8: 340. doi:10.1038/s41467-017-00421-x.

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 Creators:
Rao, Radhika G.1, 2, Author
Blume, Raoul3, Author           
Hansen, Thomas W.4, Author
Fuentes, Erika5, Author
Dreyer, Kathleen6, Author
Moldovan, Simona7, Author
Ersen, Ovidiu7, Author
Hibbitts, David D.6, Author
Chabal, Yves J.5, Author
Schlögl, Robert3, Author           
Tessonnier, Jean-Philippe1, 2, Author
Affiliations:
1Department of Chemical and Biological Engineering, Iowa State University, Ames, IA 50011, USA, ou_persistent22              
2NSF Engineering Research Center for Biorenewable Chemicals, Ames, IA 50011, USA, ou_persistent22              
3Inorganic Chemistry, Fritz Haber Institute, Max Planck Society, ou_24023              
4Center for Electron Nanoscopy, Technical University of Denmark, DK-2800 Kgs Lyngby, Denmark, ou_persistent22              
5Department of Materials Science and Engineering, University of Texas at Dallas, Richardson, TX 75080, USA, ou_persistent22              
6Department of Chemical Engineering, University of Florida, Gainesville, FL 32611, USA, ou_persistent22              
7Institut de Physique et Chimie des Matériaux de Strasbourg, UMR 7504 University of Strasbourg – CNRS, FR-67200 Strasbourg, France, ou_persistent22              

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 Abstract: Controlling the charge transfer between a semiconducting catalyst carrier and the supported transition metal active phase represents an elite strategy for fine turning the electronic structure of the catalytic centers, hence their activity and selectivity. These phenomena have been theoretically and experimentally elucidated for oxide supports but remain poorly understood for carbons due to their complex nanoscale structure. Here, we combine advanced spectroscopy and microscopy on model Pd/C samples to decouple the electronic and surface chemistry effects on catalytic performance. Our investigations reveal trends between the charge distribution at the palladium–carbon interface and the metal’s selectivity for hydrogenation of multifunctional chemicals. These electronic effects are strong enough to affect the performance of large (~5 nm) Pd particles. Our results also demonstrate how simple thermal treatments can be used to tune the interfacial charge distribution, hereby providing a strategy to rationally design carbon-supported catalysts.

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Language(s): eng - English
 Dates: 2017-03-292017-06-282017-08-24
 Publication Status: Published online
 Pages: 10
 Publishing info: -
 Table of Contents: -
 Rev. Type: Peer
 Identifiers: DOI: 10.1038/s41467-017-00421-x
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Title: Nature Communications
  Abbreviation : Nat. Commun.
Source Genre: Journal
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Publ. Info: London : Nature Publishing Group
Pages: - Volume / Issue: 8 Sequence Number: 340 Start / End Page: - Identifier: ISSN: 2041-1723
CoNE: https://pure.mpg.de/cone/journals/resource/2041-1723