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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
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

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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