Ghent University Academic Bibliography

Advanced

The remarkable amphoteric nature of defective UiO-66 in catalytic reactions

Julianna Hajek UGent, Bart Bueken, Michel Waroquier UGent, Dirk De Vos and Veronique Van Speybroeck UGent (2017) CHEMCATCHEM. 9(12). p.2203-2210
abstract
One of the major requirements in solid acid and base catalyzed reactions is that the reactants, intermediates or activated complexes cooperate with several functions of catalyst support. In this work the remarkable bifunctional behavior of the defective UiO-66(Zr) metal organic framework is shown for acid-base pair catalysis. The active site relies on the presence of coordinatively unsaturated zirconium sites, which may be tuned by removing framework linkers and by removal of water from the inorganic bricks using a dehydration treatment. To elucidate the amphoteric nature of defective UiO-66, the Oppenauer oxidation of primary alcohols has been theoretically investigated using density functional theory (DFT) and the periodic approach. The presence of acid and basic centers within molecular distances is shown to be crucial for determining the catalytic activity of the material. Hydrated and dehydrated bricks have a distinct influence on the acidity and basicity of the active sites. In any case both functions need to cooperate in a concerted way to enable the chemical transformation. Experimental results on UiO-66 materials of different defectivity support the theoretical observations made in this work.
Please use this url to cite or link to this publication:
author
organization
year
type
journalArticle (original)
publication status
published
subject
keyword
DFT, kinetics, lewis acid site, bronsted base site, catalysis
journal title
CHEMCATCHEM
volume
9
issue
12
pages
2203 - 2210
publisher
WILEY-V C H VERLAG GMBH
place of publication
WEINHEIM, GERMANY
conference name
1st French Conference on Catalysis (FCCat)
conference location
Frejus, FRANCE
conference start
2016-05-23
conference end
2016-05-27
Web of Science type
Article
Web of Science id
000404031300019
ISSN
1867-3880
1867-3899
DOI
10.1002/cctc.201601689
language
English
UGent publication?
yes
classification
A1
copyright statement
Creative Commons Attribution 4.0 International Public License (CC-BY 4.0)
id
8531598
handle
http://hdl.handle.net/1854/LU-8531598
date created
2017-09-19 07:40:54
date last changed
2017-09-22 09:39:20
@article{8531598,
  abstract     = {One of the major requirements in solid acid and base catalyzed reactions is that the reactants, intermediates or activated complexes cooperate with several functions of catalyst support. In this work the remarkable bifunctional behavior of the defective UiO-66(Zr) metal organic framework is shown for acid-base pair catalysis. The active site relies on the presence of coordinatively unsaturated zirconium sites, which may be tuned by removing framework linkers and by removal of water from the inorganic bricks using a dehydration treatment. To elucidate the amphoteric nature of defective UiO-66, the Oppenauer oxidation of primary alcohols has been theoretically investigated using density functional theory (DFT) and the periodic approach. The presence of acid and basic centers within molecular distances is shown to be crucial for determining the catalytic activity of the material. Hydrated and dehydrated bricks have a distinct influence on the acidity and basicity of the active sites. In any case both functions need to cooperate in a concerted way to enable the chemical transformation. Experimental results on UiO-66 materials of different defectivity support the theoretical observations made in this work.},
  author       = {Hajek, Julianna and Bueken, Bart and Waroquier, Michel and De Vos, Dirk and Van Speybroeck, Veronique},
  issn         = {1867-3880},
  journal      = {CHEMCATCHEM},
  keyword      = {DFT,kinetics,lewis acid site,bronsted base site,catalysis},
  language     = {eng},
  location     = {Frejus, FRANCE},
  number       = {12},
  pages        = {2203--2210},
  publisher    = {WILEY-V C H VERLAG GMBH},
  title        = {The remarkable amphoteric nature of defective UiO-66 in catalytic reactions},
  url          = {http://dx.doi.org/10.1002/cctc.201601689},
  volume       = {9},
  year         = {2017},
}

Chicago
Hajek, Julianna, Bart Bueken, Michel Waroquier, Dirk De Vos, and Veronique Van Speybroeck. 2017. “The Remarkable Amphoteric Nature of Defective UiO-66 in Catalytic Reactions.” Chemcatchem 9 (12): 2203–2210.
APA
Hajek, J., Bueken, B., Waroquier, M., De Vos, D., & Van Speybroeck, V. (2017). The remarkable amphoteric nature of defective UiO-66 in catalytic reactions. CHEMCATCHEM, 9(12), 2203–2210. Presented at the 1st French Conference on Catalysis (FCCat).
Vancouver
1.
Hajek J, Bueken B, Waroquier M, De Vos D, Van Speybroeck V. The remarkable amphoteric nature of defective UiO-66 in catalytic reactions. CHEMCATCHEM. WEINHEIM, GERMANY: WILEY-V C H VERLAG GMBH; 2017;9(12):2203–10.
MLA
Hajek, Julianna, Bart Bueken, Michel Waroquier, et al. “The Remarkable Amphoteric Nature of Defective UiO-66 in Catalytic Reactions.” CHEMCATCHEM 9.12 (2017): 2203–2210. Print.