ACS Catalysis · 2014 · 209 citations · 58 references
Natural SciencesChemical EngineeringChemistryCatalysisInorganic ChemistryNanomaterialsCatalyst CharacterizationCatalyst DeactivationCatalytic MaterialsCatalytic MechanismsNanocatalysisSupported CatalystsCatalytic ActivityElectron-withdrawing GroupsExtended X-ray Absorption Fine StructureLewis AcidityMetal-organic Framework CatalystsNanostructured CatalystsPalladium CatalystsTandem Catalysis
A bifunctional Zr-MOF catalyst containing palladium nanoclusters (NCs) has been developed. The formation of Pd NCs was confirmed by transmission electron microscopy (TEM) and extended X-ray absorption fine structure (EXAFS). Combining the oxidation activity of Pd NCs and the acetalization activity of the Lewis acid sites in UiO-66-NH 2, this catalyst (Pd@UiO-66-NH 2 ) exhibits excellent catalytic activity and selectivity in a one-pot tandem oxidation-acetalization reaction. This catalyst shows 99.9% selectivity to benzaldehyde ethylene acetal in the tandem reaction of benzyl alcohol and ethylene glycol at 99.9% conversion of benzyl alcohol. We also examined various substituted benzyl alcohols and found that alcohols with electron-donating groups showed better conversion and selectivity compared to those with electron-withdrawing groups. We further proved that there was no leaching of active catalytic species during the reaction and the catalyst can be recycled at least five times without significant deactivation.
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Multiple-scattering calculations of x-ray-absorption spectra
S. I. Zabinsky, J. J. Rehr, A. L. Ankudinov et al. · Physical review. B, Condensed matter · 1995 · 2.9K citations