Tandem Catalysis by Palladium Nanoclusters Encapsulated in Metal–Organic Frameworks

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2014-01-01
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Li, Xinle
Guo, Zhiyong
Xiao, Chaoxian
Goh, Tian Wei
Tesfagaber, Daniel
Huang, Wenyu
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Ames National LaboratoryChemistry
Abstract

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-NH2, this catalyst (Pd@UiO-66-NH2) 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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Reprinted (adapted) with permission from ACS Catal., 2014, 4 (10), pp 3490–3497). Copyright 2014 American Chemical Society.

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Wed Jan 01 00:00:00 UTC 2014
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