Molecular Origin of the Selectivity Differences between Palladium and Gold-Palladium in Benzyl Alcohol Oxidation: Different Oxygen Adsorption Properties

Savara, Aditya; Chan-Thaw, Carine E.; Sutton, Jonathan E.; Wang, Di; Prati, Laura; Villa, Alberto

doi:10.1002/cctc.201601295

Title: Molecular Origin of the Selectivity Differences between Palladium and Gold-Palladium in Benzyl Alcohol Oxidation: Different Oxygen Adsorption Properties

Journal Article · Wed Nov 02 00:00:00 EDT 2016 · ChemCatChem

DOI:https://doi.org/10.1002/cctc.201601295· OSTI ID:1344268

^[1]; Chan-Thaw, Carine E. ^[2];

^[1]; Wang, Di ^[3]; Prati, Laura ^[2];

^[2]

Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Chemical Sciences Division
Univ. degli Studi di Milano via Golgi, Milano (Italy). Dipartimento di Chimica
Karlsruhe Inst. of Technology, Eggenstein-Leopoldshafen (Germany). Inst. of Nanotechnology and Karlsruhe Nano Micro Facility

The same mechanism and microkinetic model used for benzyl alcohol oxidation over Pd/C was shown to apply to benzyl alcohol oxidation over AuPd/C. Almost all of the selectivity differences could be explained by a decrease in oxygen adsorption on AuPd. After isolating oxygen adsorption as being the origin of the selectivity differences, density functional theory was used to investigate the oxygen adsorption properties of a pure Pd surface, a pure Au surface, and an alloyed AuPd surface. Finally, the calculations showed that Au–Pd alloying decreased the oxygen adsorption properties relative to pure Pd, which explained the selectivity differences, consistent with the microkinetic modeling.

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Research Organization:: Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Oak Ridge Leadership Computing Facility (OLCF)

Sponsoring Organization:: USDOE Office of Science (SC)

Grant/Contract Number:: AC05-00OR22725

OSTI ID:: 1344268

Journal Information:: ChemCatChem, Vol. 9, Issue 2; ISSN 1867-3880

Publisher:: ChemPubSoc EuropeCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 33 works

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Au−Pd Selectivity‐switchable Alcohol‐oxidation Catalyst: Controlling the Duality of the Mechanism using a Multivariate Approach da S. Melo, Itaciara E. M.; de Sousa, Samuel A. A.; dos S. Pereira, Laíse N. ChemCatChem, Vol. 11, Issue 13 https://doi.org/10.1002/cctc.201900512	journal	June 2019
What is the effect of Sn and Mo oxides on gold catalysts for selective oxidation of benzyl alcohol? Xu, Jing; Wang, Yue; Cao, Yunxiang New Journal of Chemistry, Vol. 43, Issue 6 https://doi.org/10.1039/c8nj05642k	journal	January 2019
Metal-free catalytic oxidation of benzylic alcohols for benzaldehyde Wang, Zhiyong; Shi, Jie; Wang, Dan Reaction Chemistry & Engineering, Vol. 4, Issue 3 https://doi.org/10.1039/c8re00265g	journal	January 2019
Selective Benzyl Alcohol Oxidation over Pd Catalysts Chan-Thaw, Carine; Savara, Aditya; Villa, Alberto Catalysts, Vol. 8, Issue 10 https://doi.org/10.3390/catal8100431	journal	September 2018

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