C-H bond activation by Pd-substituted CeO 2: Substituted ions versus reduced species

Misch, Lauren M., Kurzman, Joshua A., Derk, Alan R., Kim, Young-Il, Seshadri, Ram, Metiu, Horia, McFarland, Eric W. and Stucky, Galen D. (2011) C-H bond activation by Pd-substituted CeO 2: Substituted ions versus reduced species. Chemistry of Materials, 23 24: 5432-5439. doi:10.1021/cm202709y


Author Misch, Lauren M.
Kurzman, Joshua A.
Derk, Alan R.
Kim, Young-Il
Seshadri, Ram
Metiu, Horia
McFarland, Eric W.
Stucky, Galen D.
Title C-H bond activation by Pd-substituted CeO 2: Substituted ions versus reduced species
Journal name Chemistry of Materials   Check publisher's open access policy
ISSN 0897-4756
1520-5002
Publication date 2011-12-27
Sub-type Article (original research)
DOI 10.1021/cm202709y
Open Access Status Not Open Access
Volume 23
Issue 24
Start page 5432
End page 5439
Total pages 8
Place of publication Washington, DC, United States
Publisher American Chemical Society
Language eng
Abstract Substituted metal oxides containing ionic species have been attracting a great deal of attention because of their potential ability to reduce the usage of precious metals in heterogeneous catalysts. We investigate Pd-substituted CeO 2 for C-H bond activation reactions including the partial oxidation and dry reforming of CH 4. This catalyst has been previously studied for CO oxidation, NO x reduction, and the water-gas shift reaction. Pd-substituted CeO 2, Ce 1-xPd xO 2-δ, was prepared as a powder with high surface area and a hollow sphere morphology using ultrasonic spray pyrolysis. The catalysts were extensively characterized using synchrotron X-ray diffraction and other techniques, confirming phase pure samples up to 10 mol % Pd substitution. Ce 0.95Pd 0.05O 2-δ was found to be active for partial oxidation of CH 4 around 500 °C and higher. Our studies, including postcatalytic synchrotron diffraction, suggest that the single-phase Ce 1-xPd xO 2-δ material is not the active species and that catalysis occurs instead over the reduced two-phase Pd 0/CeO 2. This observation has been further confirmed by verifying the activity of the reduced Pd 0/CeO 2 catalysts for ethylene hydrogenation, a reaction that is known to require Pd 0.
Keyword Catalyst
Hydrocarbon
Nanoparticle
Q-Index Code C1
Q-Index Status Provisional Code
Institutional Status Non-UQ

Document type: Journal Article
Sub-type: Article (original research)
Collection: School of Chemical Engineering Publications
 
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