Interfacial charge distributions in carbon-supported palladium catalysts

Date
2017-08-24
Authors
Rao, Radhika
Blume, Raoul
Hansen, Thomas
Tessonnier, Jean-Philippe
Fuentes, Erika
Dreyer, Kathleen
Moldovan, Simona
Ersen, Ovidiu
Hibbitts, David
Chabal, Yves
Schlögl, Robert
Tessonnier, Jean-Philippe
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NSF Engineering Research Center for Biorenewable ChemicalsChemical and Biological Engineering
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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This article is published as Rao, Radhika G., Raoul Blume, Thomas W. Hansen, Erika Fuentes, Kathleen Dreyer, Simona Moldovan, Ovidiu Ersen et al. "Interfacial charge distributions in carbon-supported palladium catalysts." Nature communications 8, no. 1 (2017): 340. DOI: 10.1038/s41467-017-00421-x. Posted with permission.

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