Solvent-Free Synthetic Route for Cerium(IV) Metal-Organic Frameworks with UiO-66 Architecture and Their Photocatalytic Applications.
DFT calculations
cerium
green syntheses
metal−organic frameworks
photocatalysis
Journal
ACS applied materials & interfaces
ISSN: 1944-8252
Titre abrégé: ACS Appl Mater Interfaces
Pays: United States
ID NLM: 101504991
Informations de publication
Date de publication:
04 Dec 2019
04 Dec 2019
Historique:
pubmed:
9
11
2019
medline:
9
11
2019
entrez:
9
11
2019
Statut:
ppublish
Résumé
A near solvent-free synthetic route for Ce-UiO-66 metal-organic frameworks (MOFs) is presented. The MOFs are obtained by energetically grinding the reagents, cerium ammonium nitrate (CAN) and the carboxylic linkers, in a mortar for a few minutes with the addition of a small amount of acetic acid (AcOH) as a modulator (8.75 equiv, 0.5 mL). The slurry is then transferred into a 2 mL vial and heated at 120 °C for 1 day. The MOFs have been characterized for their composition, crystallinity, and porosity and employed as heterogeneous catalysts for the photo-oxidation reaction of substituted benzylic alcohols to benzaldaldehydes under near-ultraviolet light irradiation. The catalytic performances, such as selectivity, conversion, and kinetics, exceed those of similar systems studied by chemical oxidation using similar Ce-MOFs as a catalyst. Moreover, the MOFs were found to be reusable up to three cycles without loss of activity. Density functional theory (DFT) calculations were used to fully describe the electronic structure of the best performing MOFs and to provide useful information on the catalytic activity experimentally observed.
Identifiants
pubmed: 31702892
doi: 10.1021/acsami.9b13730
doi:
Types de publication
Journal Article
Langues
eng
Sous-ensembles de citation
IM