Interfacial charge distributions in carbon-supported palladium catalysts

Radhika G. Rao, Raoul Blume, Thomas W. Hansen, Erika Fuentes, Kathleen Dreyer, Simona Moldovan, Ovidiu Ersen, David D. Hibbitts, Yves J. Chabal, Robert Schlögl and Jean-Philippe Tessonnier ()
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Radhika G. Rao: Iowa State University
Raoul Blume: Max Planck Society
Thomas W. Hansen: Technical University of Denmark
Erika Fuentes: University of Texas at Dallas
Kathleen Dreyer: University of Florida
Simona Moldovan: UMR 7504 University of Strasbourg – CNRS
Ovidiu Ersen: UMR 7504 University of Strasbourg – CNRS
David D. Hibbitts: University of Florida
Yves J. Chabal: University of Texas at Dallas
Robert Schlögl: Max Planck Society
Jean-Philippe Tessonnier: Iowa State University

Nature Communications, 2017, vol. 8, issue 1, 1-10

Abstract: 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.

Date: 2017
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DOI: 10.1038/s41467-017-00421-x

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