Tandem catalysis by palladium nanoclusters encapsulated in metal–organic frameworks
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. 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:
-
- Iowa State Univ., Ames, IA (United States); Ames Lab., Ames, IA (United States)
- Publication Date:
- Research Org.:
- Ames Laboratory (AMES), Ames, IA (United States)
- Sponsoring Org.:
- USDOE
- OSTI Identifier:
- 1225525
- Report Number(s):
- IS-J-8534
Journal ID: ISSN 2155-5435
- Grant/Contract Number:
- 200021-129511
- Resource 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
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 77 NANOSCIENCE AND NANOTECHNOLOGY; tandem catalysis; acetalization; bifunctional catalysts; UiO-66; Zr-MOF; nanoclusters; heterogeneous catalysis
Citation Formats
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., 2014.
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. https://doi.org/10.1021/cs5006635
Li, Xinle, Guo, Zhiyong, Xiao, Chaoxian, Goh, Tian Wei, Tesfagaber, Daniel, and Huang, Wenyu. Mon .
"Tandem catalysis by palladium nanoclusters encapsulated in metal–organic frameworks". United States. https://doi.org/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 = {Mon Aug 25 00:00:00 EDT 2014},
month = {Mon Aug 25 00:00:00 EDT 2014}
}
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