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Tandem Catalysis by Palladium Nanoclusters Encapsulated in Metal-Organic Frameworks

TitleTandem Catalysis by Palladium Nanoclusters Encapsulated in Metal-Organic Frameworks
Publication TypeJournal Article
Year of Publication2014
AuthorsLi, XL, Guo, ZY, Xiao, CX, Goh, TW, Tesfagaber, D, Huang, WK
JournalAcs Catalysis
Volume4
Pagination3490-3497
Date Published10
Type of ArticleArticle
ISBN Number2155-5435
Accession NumberWOS:000345735200017
Keywordsacetal, acetalization, aerobic, bifunctional catalysts, cascade reactions, formic-acid, gold clusters, heterogeneous catalyst, hydrogen-peroxide, linker substitution, multifunctional catalysts, oxidation, primary alcohols, selective oxidation, solid acid, tandem synthesis, UiO-66
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.

DOI10.1021/cs5006635
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