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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-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. 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.
Authors:
 [1] ;  [1] ;  [1] ;  [1] ;  [1] ;  [1]
  1. Iowa State Univ., Ames, IA (United States); Ames Lab., Ames, IA (United States)
Publication Date:
Report Number(s):
IS-J-8534
Journal ID: ISSN 2155-5435
Grant/Contract Number:
200021-129511
Type:
Accepted Manuscript
Journal Name:
ACS Catalysis
Additional Journal Information:
Journal Volume: 4; Journal Issue: 10; Journal ID: ISSN 2155-5435
Publisher:
American Chemical Society
Research Org:
Ames Laboratory (AMES), Ames, IA (United States)
Sponsoring Org:
USDOE
Country of Publication:
United States
Language:
English
Subject:
77 NANOSCIENCE AND NANOTECHNOLOGY; tandem catalysis; acetalization; bifunctional catalysts; UiO-66; Zr-MOF; nanoclusters; heterogeneous catalysis
OSTI Identifier:
1225525

Li, Xinle, Guo, Zhiyong, Xiao, Chaoxian, Goh, Tian Wei, Tesfagaber, Daniel, and Huang, Wenyu. Tandem catalysis by palladium nanoclusters encapsulated in metal–organic frameworks. United States: N. p., Web. doi:10.1021/cs5006635.
Li, Xinle, Guo, Zhiyong, Xiao, Chaoxian, Goh, Tian Wei, Tesfagaber, Daniel, & Huang, Wenyu. Tandem catalysis by palladium nanoclusters encapsulated in metal–organic frameworks. United States. doi:10.1021/cs5006635.
Li, Xinle, Guo, Zhiyong, Xiao, Chaoxian, Goh, Tian Wei, Tesfagaber, Daniel, and Huang, Wenyu. 2014. "Tandem catalysis by palladium nanoclusters encapsulated in metal–organic frameworks". United States. doi:10.1021/cs5006635. https://www.osti.gov/servlets/purl/1225525.
@article{osti_1225525,
title = {Tandem catalysis by palladium nanoclusters encapsulated in metal–organic frameworks},
author = {Li, Xinle and Guo, Zhiyong and Xiao, Chaoxian and Goh, Tian Wei and Tesfagaber, Daniel and Huang, Wenyu},
abstractNote = {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.},
doi = {10.1021/cs5006635},
journal = {ACS Catalysis},
number = 10,
volume = 4,
place = {United States},
year = {2014},
month = {8}
}