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Title: Tandem catalysis by palladium nanoclusters encapsulated in metal–organic frameworks

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. As a result, 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.
 [1] ;  [1] ;  [1] ;  [1] ;  [1] ;  [1]
  1. Iowa State Univ., Ames, IA (United States); Ames Lab., Ames, IA (United States)
Publication Date:
OSTI Identifier:
Report Number(s):
Journal ID: ISSN 2155-5435
Grant/Contract Number:
Accepted Manuscript
Journal Name:
ACS Catalysis
Additional Journal Information:
Journal Volume: 4; Journal Issue: 10; Journal ID: ISSN 2155-5435
American Chemical Society
Research Org:
Ames Laboratory (AMES), Ames, IA (United States)
Sponsoring Org:
Country of Publication:
United States
77 NANOSCIENCE AND NANOTECHNOLOGY tandem catalysis; acetalization; bifunctional catalysts; UiO-66; Zr-MOF; nanoclusters; heterogeneous catalysis